a guided walk through larry hench’s monumental...
TRANSCRIPT
IN HONOR OF LARRY HENCH
A guided walk through Larry Hench’s monumental
discoveries
Maziar Montazerian1,* and Edgar D. Zanotto1,*
1Department of Materials Engineering (DEMa), Center for Research, Technology and Education in Vitreous Materials (CeRTEV),
Federal University of São Carlos (UFSCar), São Carlos, SP 13.565-905, Brazil
Received: 23 September 2016
Accepted: 16 January 2017
� Springer Science+Business
Media New York 2017
ABSTRACT
Here we review and summarize the groundbreaking scientific researches of the
late Professor Larry L. Hench, including several of his key discoveries in
materials science and engineering. First, we provide a statistical overview of his
exceptional scientific performance using Scopus, Web of Science, and other Web
sites to extract statistical data on his scientific publications and patents. Pro-
fessor Hench achieved an exceptionally high h-index of 77 (Scopus) for the field
of materials science and engineering, which resulted from his 340 research
papers, 210 conference papers, 41 patents, 24 books, 4 editorial notes, and 3
biographies starting in 1967. Then, we summarize and highlight his seminal
articles, books, and patents in several research areas, such as bioactive glasses,
optical gel glasses, biocomposites/coatings, glass–ceramics, biophotonics,
advanced ceramics, semiconducting and ionic conducting glasses, glass corro-
sion, and nuclear waste disposal. Prof. Hench not only discovered the first man-
made material to form a chemical bond with bone and initiated a whole new
field—bioactive glasses and glass–ceramics—but also made several other
important scientific discoveries. It is quite clear that he was one of the most
influential materials scientists/engineers of all time! We hope that this review is
not only useful for all persons interested in materials science and engineering
but also encourages students and younger investigators to make use of this
accumulated knowledge to design novel materials and discover new applica-
tions for glasses and ceramics.
Hench by the numbers
Hench’s publications have been indexed in the Web
of Science since 1967 [1]. He published an average of
12 articles per year [1]. He also wrote or edited
approximately one book every 2 years [2]. Professor
Hench’s h-index at Scopus is 77 [3], resulting from
the publication of approximately 340 research papers
[1], 210 conference papers [1], 41 patents [1], 24 books
[2], 20 review papers [1], 23 book chapters [3], 4
editorial notes [1], 2 letters [1], and 3 biographies [1],
which lead to a total of 25,753 citations until July
Address correspondence to E-mail: [email protected]; [email protected]
DOI 10.1007/s10853-017-0804-4
J Mater Sci
In Honor of Larry Hench
2016. Figure 1 shows his number of publications and
citations.
Hench performed research in the fields of materials
science and engineering, chemistry, biochemistry,
genetics, biology, physics, medicine, and dentistry.
The research subjects tackled and his publication
quantity in each subject are summarized in Fig. 2.
Hench’s scientific papers have been published in
several materials science and engineering journals
(Fig. 3). He was also a member of the editorial advi-
sory boards of some of them. His publications are
highly cited and are key references for engineers and
scientists of various interdisciplinary fields. Lists of
his books and highly cited papers are given in
Tables 1 and 2, respectively.
Our statistical analysis of Hench’s work and pub-
lications revealed that his main research subjects
were bioactive glasses, optical gel glasses, biocom-
posites/coatings, glass–ceramics, advanced ceramics,
semiconducting and ionic conducting glasses, glass
corrosion, and nuclear waste disposal. Therefore, in
this article, we highlight his main discoveries in these
areas.
Bioactive glasses (Refs. [32, 44, 50–238])
Without any doubt, the discovery in 1969 of the first
man-made biomaterial that could bond to living bone
and tissues was Hench’s most monumental discovery
3
15
16
21
23
29
34
36
37
45
82
217
0 40 80 120 160 200 240
Obituaries
Waste forms
Bioac�ve coa�ngs
Semi/ion-conduc�ng glasses
Bio-photonics
Glass-ceramics
Bio-composites
Review papers on biomaterials
Advanced ceramics
Glass corrosion and leaching
Op�cal gel-glasses
Bioac�ve glasses
Number of Publica�ons
Figure 2 Main research
subjects investigated by Hench
and the number of publications
in each, including
journal/conference papers and
patents [1].
0
6
12
18
24
30
36
42
0
300
600
900
1200
1500
1800
2100
Num
ber o
f Pub
lica�
ons
Cita
�ons
Year
Figure 1 Hench’s
publications and citations per
year [1, 3] until July 2016.
J Mater Sci
[35]. In the summer of 1967, he had the good fortune
of talking to an army officer on a bus ride during his
return from a conference. They discussed the tragic
result during the Vietnam War of wounds to limbs of
soldiers that shattered only a portion of the limb but
required amputation of the entire limb because of the
3 3 3 3 3 4 5 6 7
9 9 10
12 12
22 42 43
58 78
0 10 20 30 40 50 60 70 80 90
ScienceJournal of the European Ceramic Society
Physics and Chemistry of GlassesJournal of the Electrochemical Society
Journal of Applied PhysicsMaterials Science Forum
Journal of Nuclear MaterialsCeramics Interna�onal
Nuclear and Chemical Waste ManagementBiomaterials Ar�ficial Organs and Tissue Engineering
Journal of Sol Gel Science and TechnologyJournal of Materials Science
Journal of Materials Science Materials in MedicineBiomaterials
Journal of the American Ceramic SocietyJournal of Non-Crystalline Solids
Key Engineering MaterialsJournal of Biomedical Materials Research (Part A & B)
American Ceramic Society Bulle�n
Number of Publica�ons
Figure 3 Hench’s quantity of
publications in 20 journals
[1, 3].
Table 1 Hench’s books [2]
No. Title Authors/editors Year Ref.
1 A biography of Bioglass L.L. Hench 2015 [4]
2 Boing–Boing the bionic cat and the Amazon Crisis L.L. Hench 2015 [5]
3 An introduction to bioceramics (2nd Edition) L.L. Hench 2013 [6]
4 Boing–Boing the bionic cat and the space station L.L. Hench 2011 [7]
5 Boing–Boing the bionic cat and the Mummy’s revenge L.L. Hench 2011 [8]
6 New materials and technologies for healthcare L.L. Hench, J.R. Jones, M.B. Fenn 2011 [9]
7 Biomaterials, artificial organs and tissue engineering L.L. Hench, J.R. Jones 2005 [10]
8 Boing–Boing the bionic cat and the flying trapeze L.L. Hench 2004 [11]
9 Boing–Boing the bionic cat and the lion’s claws L.L. Hench 2004 [12]
10 Future strategies for tissue & organ replacement J.M. Polak, L.L. Hench, P. Kemp 2002 [13]
11 Science, faith and ethics L.L. Hench 2002 [14]
12 Boing–Boing: the bionic cat and the jewel thief L.L. Hench 2001 [15]
13 Boing–Boing the Bionic cat L.L. Hench 2000 [16]
14 Sol–gel silica: properties, processing and technology transfer L.L. Hench 1998 [17]
15 Bioceramics, vol 8 J. Wilson, L.L. Hench, D. Greenspan 1995 [18]
16 Clinical performance of skeletal prostheses J. Wilson, L.L. Hench 1995 [19]
17 Chemical processing of advanced materials L.L. Hench and J.K. West 1992 [20]
18 CRC handbook of bioactive ceramics, vol I T. Yamamuro, L.L. Hench, J. Wilson 1990 [21]
19 CRC handbook of bioactive ceramics, vol II T. Yamamuro, L.L. Hench, J. Wilson 1990 [22]
20 Principles of electronic ceramics L.L. Hench, J.K. West 1990 [23]
21 Science of ceramic chemical processing L.L. Hench, D.R. Ulrich 1986 [24]
22 Ultrastructure processing of ceramics, glasses, and composites L.L. Hench, D.R. Ulrich 1984 [25]
23 Ceramic processing before firing L. L. Hench, G.Y. Onoda 1978 [26]
24 Bibliography on ceramics and glass L.L. Hench, B.A. McEldowney 1976 [27]
J Mater Sci
lack of supporting/replacing material for bone.
Hench formulated a sodium–calcium–phosphorous–
silicate composition in which the ratio of Ca/P
mimics the stoichiometry of Ca/P in bone. He tried a
handful of compositions based on the SiO2–Na2O–
CaO phase diagram and came up with the 45SiO2–
24.5CaO–24.5Na2O–6P2O5 (wt%) glass composition,
known as 45S5 Bioglass�, proving its bone-bonding
ability. This invention opened up a whole new field—
‘‘bioactive glasses’’—in which the principal goal was
to develop, test, and use materials that bond to bone.
With careful studies, primary assistance from Drs.
Splinter, Greenlee, and Allen [32], who were ortho-
pedists, and shortly after with Drs. G. Miller, G.
Piotrowski, A.E. Clark, and D.C. Greenspan, and
support from the US Army Medical R&D Command,
Hench achieved this seminal discovery [35].
Bioactive glasses undergo a particular biological
reaction at the interface, which stimulates cell pro-
liferation, gene response and the formation of a bond
between living tissues and the material. A common
feature of bioactive glasses is that their surface
develops a biologically active hydroxycarbonate
apatite (HCA) layer that bonds to bone. The HCA
phase that forms on these glasses is chemically and
structurally equivalent to the mineral phase of bone
and teeth. This similarity is key for interfacial bond-
ing [35].
This discovery opened up a totally new interdis-
ciplinary area in materials science and engineering,
chemistry, biochemistry, medicine, dentistry and
biology. There are dozens of conferences and scien-
tific journals currently dealing with biomaterials; one
journal is specifically dedicated to Hench’s discovery,
Biomedical Glasses.
Hench and his students and colleagues managed to
license their inventions to companies that commer-
cialized the bioactive glass 45S5 Bioglass� for dental
and medical applications. Bioglass�-derived products
include Perioglas�, NovaBone�, and NovaMin�
Table 2 Hench’s most cited papers [3] until July 2016
No. Title Year Citations Ref.
1 Bioceramics: from concept to clinic 1991 3097 [28]
2 The sol–gel process 1990 2496 [29]
3 Bioceramics 1998 1976 [30]
4 Third-generation biomedical materials 2002 1344 [31]
5 Bonding mechanisms at the interface of ceramic prosthetic materials 1971 773 [32]
6 Gene-expression profiling of human osteoblasts following treatment with the ionic products of Bioglass�
45S5 dissolution
2001 652 [33]
7 Surface-active biomaterials 1984 629 [34]
8 The story of Bioglass� 2006 626 [35]
9 Ionic products of bioactive glass dissolution increase proliferation of human osteoblasts and induce insulin-
like growth factor II mRNA expression and protein synthesis
2000 499 [36]
10 Bioactive materials 1996 471 [37]
11 Biomaterials: a forecast for the future 1998 429 [38]
12 Direct chemical bond of bioactive glass ceramic materials to bone and muscle 1973 420 [39]
13 Bioglass� 45S5 stimulates osteoblast turnover and enhances bone formation in vitro: implications and
applications for bone tissue engineering
2000 397 [40]
14 Optimising bioactive glass scaffolds for bone tissue engineering 2006 333 [41]
15 An investigation of bioactive glass powders by sol–gel processing 1991 312 [42]
16 Highly bioactive P2O5–Na2O–CaO–SiO2 glass–ceramics 2001 284 [43]
17 Calcium phosphate formation on sol–gel-derived bioactive glasses in vitro 1994 253 [44]
18 Nodule formation and mineralisation of human primary osteoblasts cultured on a porous bioactive glass
scaffold
2004 248 [45]
19 Effect of crystallization on apatite-layer formation of bioactive glass 45S5 1996 244 [46]
20 Toxicology and biocompatibility of bioglasses 1981 228 [47]
21 Development and in vitro characterisation of novel bioresorbable and bioactive composite materials based
on polylactide foams and Bioglass� for tissue engineering applications
2002 228 [48]
22 Bioactive materials: the potential for tissue regeneration 1998 210 [49]
J Mater Sci
(Fig. 4). These products and some cones of Bioglass�
were used clinically as ossicular reconstruction pros-
theses, endosseous ridge maintenance implants, bone
grafts to restore bone loss from periodontal disease in
infrabony defects, bone grafts in tooth extraction sites
and alveolar ridge augmentation, and orthopedic bone
grafting in general [35]. Now, Bioglass� is used as a
coarse particulate for bone grafting, fine particulate in
Sensodyne� toothpaste for dentinal hypersensitivity
treatment (NovaMin�), and as some custom implants.
There is a recent commercial use for Bioglass� as afiber
composite (Bio2 Technologies, Inc.), but the ossicular
replacement and endosseous implant apparently are
no longer in use [50].
Hench published more than 200 papers, book
chapters and patents specifically dealing with his
bioactive glass [1]. Forty-seven years after the intro-
duction of bioactive glasses, more than 5,000 publica-
tions describe in vitro, in vivo or clinical performance
of 45S5, other bioactive glasses and glass–ceramics [1].
Fortunately, during his lifetime, he reviewed the
history, processing, properties and applications of
bioactive glasses. He demonstrated a successful path
from a brand new concept to applications, which are
still wide open to future innovations. Hench came up
with the concept of the bone-bonding ability of certain
glasses. Then, hemanaged to apply this idea to clinical
applications and finally opened a new era of research
for gene-activating glasses [180, 214, 216–218, 222, 223].
The objective of this paper is not merely reviewing
Hench’s achievements in this field because his own
review papers are very comprehensive. What we
intend to accomplish here is to list and comment on
his key review papers (see Table 3) to guide and
encourage the interested reader in their study. For
example, in the highly cited paper ‘‘The story of
Bioglass�’’ [35], Hench describes the story of a sec-
ond-generation biomaterial, Bioglass�, as an exciting
alternative for the first-generation inert biomaterials.
The steps of discovery, characterization, in vitro and
in vivo evaluations, clinical studies, and product
development are elegantly summarized along with
the technology transfer processes [35]. Then, Hench
and Julia Polak [31] called attention to the gene-acti-
vating properties of bioactive glasses, which became
known as the third generation of biomaterials for
tissue regeneration and repair [31]. They established
the Tissue Engineering and Regenerative Medicine
Centre (TERM) at Imperial College London to pro-
mote collaboration between biologists and materials
scientists. Early works at their centre elucidated the
beneficial interactions between primary human
Figure 4 Bioactive glass products for a periodontal disease therapy (Perioglas�), b orthopedic bone grafting (NovaBone�) and
c particulates in toothpaste for dentinal hypersensitivity treatment (NovaMin�).
J Mater Sci
osteoblasts and 45S5 Bioglass� (Fig. 5). Then, the
team discovered that the dissolution products of
bioactive glasses have osteoblastic stimulatory and
gene-activating properties. This extensive research on
bioactive glasses proved their suitability when
assembled as scaffolds for bone tissue engineering, as
they not only provide an osteoconductive and
osteoproductive substrate—which is due to ion
release from the glass—but also actively stimulate
cells to express appropriate osteoblastic phenotypes
[40]. Therefore, they came to the conclusion that ‘‘a
cellular and molecular basis for development of
third-generation biomaterials provides the scientific
foundation for molecular design of scaffolds for tis-
sue engineering and for in situ tissue regeneration
and repair, with minimally invasive surgery. Impor-
tant economic advantages to each of these new
approaches may aid in solving the problems of caring
for an aging population’’ [31].
Finally, Professor Hench inspired many scientists
with his famous phrase: ‘‘…avoid pursuing small
incremental advancements in this exciting field.
Instead, researchers should strive for unique and
innovative approaches at a fundamental molecular
biology level to create new bioactive materials and
test them in representative biological conditions that
mimic their use clinically. The goal must be to create
materials that are revolutionary and can improve the
quality of life and care for our aging population
without increasing the cost of care. This is a goal
worth striving for and a vision that will last for
decades’’ [223].
Larry Hench also introduced the first gel-derived
highly bioactive glasses in 1991. He and his Ph.D
students, Li and Pereira, in their highly cited papers
[42, 44] studied different compositions and per-
formed in vitro bioactivity tests in simulated body
fluid. Surprisingly, gel-derived glasses with nearly
Table 3 Hench’s seminal review papers on bioactive glasses
No. Title Year Refs.
1 Bioglass: 10 milestones from concept to commerce 2016 [222]
2 Opening paper 2015—some comments on Bioglass�: four eras of discovery and development 2015 [223]
3 Bioactive glasses beyond bone and teeth: emerging applications in contact with soft tissues 2015 [220]
4 Chronology of bioactive glass development and clinical applications 2013 [218]
5 Interactions between bioactive glass and collagen: a review and new perspectives 2013 [217]
6 Glass and medicine 2010 [216]
7 Genetic design of bioactive glass 2009 [214]
8 The story of Bioglass� 2006 [35]
9 Bioactive glasses for in situ tissue regeneration 2004 [180]
10 Third-generation biomedical materials 2002 [31]
Figure 5 a Scanning electron micrograph of a human primary
osteoblast cultured on a 45S5 Bioglass� disk for 2 days.
b Osteoblast in contact with 45S5 Bioglass� disk after 6 days in
culture. The osteoblast has assumed a more flattened morphology
and is anchored to the substrate by multiple lamellipodia. Modified
from Ref. [40], with permission from Springer.
J Mater Sci
90 mol% SiO2 were found to be bioactive (the bioac-
tive melt-derived glasses generally have less than
55 mol% SiO2). The rate of surface hydroxycarbonate
apatite (HCA) formation was higher than in melt-
derived glasses of the same composition. This finding
suggested a promising chemistry-based method for
the molecular and textural design of new bioactive
glasses. The sol–gel method also made it possible to
control the size and distribution of mesopores and
macropores in ranges 2–50 nm and 100–500 lm,
respectively [120, 124]. In the early 2000s, bioactive
gel glass compositions were simplified by Saravana-
pavan and Hench to just two components (CaO and
SiO2). They showed that the gel-derived 70SiO2–
30CaO (in mol%) glass was as bioactive as the gel-
derived 58S (60SiO2–36CaO–4P2O5 in mol%) or melt-
derived 45S5 Bioglass� [145, 173, 190]. This CaO–SiO2
system was the basis for many of Hench’s studies on
tissue regeneration. Then, the performances of gel-
derived glasses were compared with melt-derived
ones by Sepulveda, Jones, and Hench [147, 158].
Meanwhile, bioactive gel glasses with silver in their
composition were also developed by Bellantone,
Coleman and Hench [142, 233]. These bioactive gel-
derived materials released silver ions at the parts per
million levels. The silver ions provided bacteriostatic
and bactericidal effects without damaging human
cells. Clinical applications in wound dressings were
then pursued [142, 233]. Finally, new gel-derived and
gene-activating bioactive glasses started to emerge.
Hench’s students and collaborators are still publish-
ing a series of papers documenting these develop-
ments. They are testing the use of sol–gel process to
produce bioactive particles, fibers, foams, porous
scaffolds, coatings, substrates, and net shape mono-
liths, which offer molecular control over the incor-
poration and biological behavior of proteins and cells
with broad applications as implants and biological
sensors [239]. The interested reader can follow vari-
ous advances and improvements in this exciting field
in the review papers authored by Jones [239],
Miguez-Pacheco et al. [221], Greenspan [240, 241],
Gentleman and Polak [242], and Woodard [243].
Optical gel glasses (Refs. [244–321])
Hench’s odyssey in the field of optical gel glasses
began 10 years after the introduction of Bioglass�
and ended with a commercial technology for
chemical processing of net shape optics. In 1979,
while visiting Professor Jerzy Zarzycki’s laboratory at
the University of Montpellier, France, Hench
observed a large (20 cm) rod of pure vitreous silica
made by sintering a hydrothermally processed xero-
gel. He was surprised to find a rod molded in its final
shape that was densified at a much lower tempera-
ture than the liquidus of pure SiO2. After returning to
the USA, he changed the focus of his laboratory from
glass surface chemistry to sol–gel processing of
glasses. His objective was to develop and commer-
cialize net shape glasses made by the sol–gel route. In
his long journey, Hench benefited from fruitful col-
laboration with and support of Dr. Donald Ulrich in
the US Air Force Office of Scientific Research
(AFOSR) [17].
Hench and his French collaborators pioneered a
particular low-temperature sol–gel process for the
rapid fabrication of large monolithic optical glasses
[17, 25, 29]. Until 1982, it was difficult to produce gel
monoliths rapidly and reliably at ambient conditions
because of the lack of control over the drying stage,
which led to cracking. Hench’s earliest studies
(1981–1984) were in collaboration between his group
(Drs. Wang and Orcel) and Professor Zarzycki’s
group (Drs. Prassas and Phalippou)
[244, 247, 255–259]. They included organic additives
(e.g., formamide (NH2CHO), glycerol (C3H8O3), and
several organic acids) in alkoxide sols to control the
rate of hydrolysis and condensation, pore size dis-
tribution, pore liquor vapor pressure, and drying
stresses. By use of proprietary drying control addi-
tives, a wide range of sizes and shapes of optically
transparent dried gel monoliths of SiO2, Na2O–SiO2,
TiO2–SiO2, LiO2–A12O3–SiO2–TiO2, and other ternary
and quaternary systems were made within a few
days at ambient atmosphere. Crack-free pieces of
dense (type V) or optically transparent nanoporous
(type VI) silica glasses were obtained after a unique
thermal stabilization or densification [29]. For exam-
ple, fully dense alkali-silicate glasses of (3–40)Na2O–
(60–97)SiO2 mol% were prepared at ambient pres-
sures from sol–gel compositions. The densification
temperatures ranged from 600 �C for high silica
glasses to 480 �C for glasses with 60–85 mol% silica
[17].
While the dense and net shape type V silica was
suggested for a variety of applications, such as opti-
cal windows, Hench’s impetus for developing a new
generation of nanoporous gel–silica matrices was the
J Mater Sci
need for a material suited for surface laser densifi-
cation of optical channel waveguides, as well as for
the impregnation of optically active organic mole-
cules. In the following years, he managed to suc-
cessfully develop micro-lenses with a homogeneous
refractive index over a large zone by selective laser
densification of gel–silica substrates containing
nanosized pores (3.2–4.5 nm). Additionally, impreg-
nation of nanoporous (4.5–9 nm) gel–silica matrices
with optically active organic molecules provided one
alternative to the production of optical composites.
Figure 6 shows the products developed by Hench for
the above applications [261, 269, 287].
In his numerous reviews on this particular subject
[261, 263, 269, 277, 287], Hench suggested the process
control variables for gel–silica optics and utilized
advanced analysis methods to show us how and why
the thermal-chemical processing works at a molecu-
lar level. Furthermore, his and J.K. West’s studies on
quantum molecular orbital (MO) modelling yielded
significant insight into the understanding of struc-
ture–property relationships for bulk amorphous sil-
ica, as well as for porous type VI gel–silica. The same
MO methods were applied by Hench and co-workers
to a variety of topics: quantum clusters of Si–SiO2,
silica densification, silica–water interactions, silica
pore models, Cr3?-doped silica, silica fracture, bio-
logical interactions of Bioglass�, and biomimetic
synthesis [102, 104, 107, 113, 119, 289, 294–296,
302–304].
The applications of the new generation of silica
optics that resulted from Hench’s investigations were
copious, such as net shape transmissive optical
elements, surface diffractive optics, inorganic doped
GRIN (gradient refractive index) optics, organic
impregnated optical hybrids such as dye lasers and
scintillators, optics with internal diffraction gratings,
laser-densified micro-optical lenses and arrays, and
laser-densified waveguides [287]. Geltech Inc., run by
his former student, Jean-Luc Nogues, was acquired
by Lightpath Technologies in the early 1990s and
produced near-net-shape optical gel glasses. Hench
summarized 15 years of sol–gel processing research
and hundreds of papers that led to the successful
commercial development of gel–silica optics in his
book titled ‘‘Sol–gel silica: properties, processing and
technology transfer’’ [17]. This book describes the key
experiments in optimizing the processing stages
involved in making stable gel-derived optical glasses
[17].
Biocomposites and coatings (Refs.[322–372])
The low fracture toughness and strength of bioactive
glasses limited their applications to low load-bearing
implants. In 1973, Hench envisaged the development
of composites for improving mechanical properties
[322]. First, Greenspan and Hench reported the first
use of Al2O3 particles to reinforce Bioglass� [323].
However, this approach did not work and led to the
first Bioglass� related patent, ‘‘Bioglass�-coated
Al2O3 ceramics’’ [370]. This coating was technically
successful but never commercialized. Then, Duch-
eyne and Hench introduced stainless steel fibers into
Figure 6 a Net shape, type V
gel glass optical windows,
b optically transparent
nanoporous type VI gel–silica
Reproduced from Ref. [269],
with permission from Elsevier.
J Mater Sci
Bioglass� by immersion of premade porous fiber
skeletons into molten glass [324]. Metal fiber rein-
forcement effectively transformed bioactive glass into
a structurally reliable material. Both strength and
toughness were higher than the properties of the
parent glass [324]. The in vivo bone-bonding ability
of the Bioglass�–stainless steel composite was
promising, and it could be deformed, subjected to
tensile stresses, machined, survived from impact
loading and, finally, presented the possibility of
preventing bacterial ingress due to its direct chemical
bonding to surrounding tissues [325]. These positive
results led to a patent registration [352].
Furthermore, Hench and his collaborators exten-
sively worked on biopolymer/Bioglass� composites.
The objective was to either reinforce/coat biopoly-
mers or trigger specific biological responses in poly-
meric bone grafts, scaffolds or cell culture plates.
They employed polysulfone [327, 349, 351], poly-
ethylene [328], polysaccharide [331], dextran [332],
polylactide [48, 335], various polymer fibers woven or
knitted into 3D patterns [333, 334, 340] and poly(dl-
lactic acid) [337, 338, 350]. As an example, an opti-
mized processing technique for the fabrication of
composites formed by polyglactin polydioxanone 3D
mesh (Ethisorb�) and Bioglass� particles has been
developed by Stamboulis et al. [333]. The procedure
was based on a powder-pressing technique [330] or
the immersion of 3D polymeric mesh into the Bio-
glass� slurry [333]. The controlled formation and
homogeneous structure and thickness of the bioactive
glass coating on the biodegradable polymer substrate
led to tailoring of the desired degradation times and
biocompatibility needed for a resorbable bioactive
tissue engineering scaffold [333]. Data on the bio-
logical response of similar composites, using resorb-
able sutures as the polymeric component, confirmed
that the bioactive glass layer could be used to control
the rate and extent of degradation of the polymers
[334]. Furthermore, the addition of medium molecu-
lar weight dextran (a complex branched glucan)
modified the glass particulate to a putty consistency
and improved the handling characteristics for use in
augmenting certain bony surfaces, i.e., large or
pleomorphic defects [332, 336]. The addition of dex-
tran did not change the bioactive properties of Bio-
glass� and had no unfavorable effects on the
ingrowth of bone into the defect sites. This composite
was patented for eventual applications [354, 356].
Bone bridges, lacy calcification and osteoblastic
activity without any histological evidence of tissue
toxicity were seen after 1 week of in vivo interaction
of Bioglass�/dextran composite with bone (Fig. 7a).
At 3 weeks, bone with an emerging trabecular pat-
tern enclosing Bioglass� particles extended across the
defects (Fig. 7b). At 6 and 12 weeks, bone remod-
elling continued and only fragments of Bioglass�
remained (Fig. 7c).
In addition to the conventional development of
Bioglass�/polymer composites, a more promising
and advanced approach that was further pursued by
his collaborators—Boccaccini, Jones, Brennan,
Figure 7 Bioglass�/dextran composite filling a rabbit bone defect
in the knee joint: a after 1 week, b after 6 weeks and c after
12 weeks. The circles show the position of the bone defect where
tested materials were placed. Samples stained with Sandersons and
Van Gieson, and magnification is 910 [332].
J Mater Sci
Pereira, Kasuga, Nazhat, Orefice, Roether, Maeda
and Gough—was to design inorganic–organic
hybrids [335, 341, 343–347]. They could form an
inorganic network of bioactive glass around
biopolymer molecules through a sol–gel process. This
resulted in molecular-level interactions of glass con-
stituents with organic compounds. These molecular-
scale interactions between the glass and polymer
components led to controlled bioactivity and the
potential to improve mechanical properties. This
open and interesting field is still followed by Hench’s
collaborators and has been thoroughly reviewed by
one of them, Jones [239].
Another approach followed by Hench to solve the
mechanical limitations of bioactive glasses and
ceramics for load-bearing applications was to apply
bioactive glasses, e.g., Bioglass�, as a coating on a
mechanically tough substrate [357–372]. Stainless
steel, cobalt–chromium, titanium alloys, and alumina
implants were commonly used as substrates. Various
techniques were utilized to deposit bioactive glass
coatings on metal implants, including plasma or
flame spraying, frit enamelling, electrophoretic
deposition and sol–gel deposition [357–372]. Details
of the development of bioactive glass coatings on
various implants are given by Hench in the first
edition of his book ‘‘An Introduction to Bioceramics’’
[6] and references [357–367]. Hench also performed
in vivo tests and registered several patents for his
novel coatings [368–372]. However, clinical applica-
tions have not been successful for the two following
main reasons: (1) The open structure of glass facili-
tates the diffusion of elements, such as Fe, Cr, Ni, Co,
Ti, or Al, to pass through the glass and change the
surface reactivity. Only a few percent of these ele-
ments is enough to make a glass non-bioactive and
stop the formation of HCA. See Ref. [82] for a review
of these compositional factors. (2) Difficulty in
achieving long-term stability of the glass–implant
interface, even though the glass is bonded to bone,
was another main drawback [6]. Therefore, to the best
of our knowledge, these inventions have not reached
the market yet.
Glass–ceramics (Refs. [373–402])
Hench’s studies on glass crystallization date back to
his M.Sc. thesis, which was supported by Owens-
Illinois Co. His proposal for the O-I fellowship was to
study the molecular mechanisms involved in the
formation of the crystalline phases in glass–ceramics
[35]. He investigated the use of dielectric relaxation
spectroscopy to follow changes in the dielectric losses
of mobile Li? cations in lithium disilicate glasses that
became much more immobile when they were
incorporated into Li2Si2O5 crystals [373–376]. Later,
under the supervision of Hench, Donald Kinser and
Stephen Freiman focused on the crystallization
kinetics and electrical and mechanical properties of
model lithium disilicate (Li2O–2SiO2) glass–ceramics.
The series of papers resulting from their Ph.D dis-
sertations provided insight for further investigations
[373–390]. Additionally, Hench was one of the first
scientists who used advanced analysis methods, such
as small angle X-ray scattering (SAXS) [385], trans-
mission electron microscopy (TEM) [388], Auger
electron spectroscopy (AES) [392], and Fourier
transform infrared spectroscopy (FTIR) [397], in the
field of glass science and technology.
In the mid-1990s, a new milestone in his research
was started with his Brazilian collaborators. In that
time, a great challenge was the development of a new
material that could combine both the high bioactivity
of Hench’s Bioglass� and the better fracture strength
and strength of some bioactive glass–ceramics, such
as Ceravital� (apatite-based glass–ceramic) and Cer-
abone� (apatite–wollastonite glass–ceramic)
[398, 399]. A straightforward strategy to achieve this
goal was via controlled crystallization of Bioglass�.
However, at that stage, the bioactive glass commu-
nity was assuming that crystallization of any glass
would impair bioactivity. Therefore, Hench and his
collaborators tried to answer two questions: (1) does
crystallization really impair bioactivity? (2) Can
crystallization of such bioactive glasses significantly
improve their mechanical properties?
Under the supervision of Larry Hench and Edgar
Zanotto, Oscar Peitl carried out his Ph.D thesis and
published two groundbreaking reports [43, 46]
demonstrating that crystallization of Bioglass�
slightly decreased the kinetics of HCA formation but
did not inhibit its formation, even in the case of full
crystallization. They demonstrated the in vitro
bioactivity of glass–ceramics with different compo-
sitions, e.g., 23.75Na2O–23.75CaO–48.5SiO2–4P2O5
(wt%), and crystallized fractions [43]. The result was
similar: crystallization did not hinder HCA formation
for glasses of this system. Later, they showed that
controlled crystallization of glasses of this system
J Mater Sci
could increase their average four-point bending
strength from 75 to 210 MPa [401]. This value is
similar to that of Cerabone� (215 MPa). The elastic
modulus also underwent a small increase, from 60 to
80 GPa, but it is still the closest value to that of
human cortical bone (*20 GPa) among the com-
mercial bioactive glass–ceramics. In addition, the
fracture toughness increased by 60% due to a crack
deflection mechanism. A patent was granted to
Hench, Peitl and Zanotto’s invention, and they called
this new material Biosilicate� [403]. They claimed the
use of this glass–ceramic in dentistry and orthopedics
[400]. Biosilicate� was found to exhibit fair machin-
ability because it is relatively easy to cut and drill,
which is an important feature that allows the fabri-
cation of implants with different shapes for specific
purposes. Before testing the effectiveness of Biosili-
cate� in clinical trials, Zanotto’s group in Brazil per-
formed a series of in vitro and in vivo studies, which
have been described elsewhere [398, 403]. Biosilicate�
is being clinically tested in dentistry for dentinal
hypersensitivity treatment, in ophthalmology as
orbital implants and in otorhinolaryngology as mid-
dle-ear ossicle implants [403]. Figure 8 shows pieces
of Biosilicate� for ossicular replacement. Otosilicate�
(the name given to these special shapes of monolithic
Biosilicate� pieces) prosthesis is an effective sub-
stituent for ossicles, not only for its biological prop-
erties but also for its machinability [403].
Furthermore, Chen et al. [404] developed three-di-
mensional (3D), highly porous, mechanically com-
petent, bioactive, and biodegradable scaffolds by the
replication technique using Bioglass� powder. Their
important finding, which confirmed the Hench,
Zanotto, and Peitl’s results [400, 401], was that the
mechanically strong crystalline phase Na2Ca2Si3O9
can transform into an amorphous calcium phosphate
phase after immersion in simulated body fluid for
28 days, and that the transformation kinetics can be
tailored through controlling the crystallinity of the
sintered 45S5 Bioglass�. Therefore, the goal of
developing a scaffold that provides good mechanical
support temporarily while maintaining bioactivity
and that biodegrades at later stages at a tailorable rate
was achieved with their Bioglass�-based scaffolds
[404].
Biophotonics (Refs. [405–428])
There has been an increasing need for noninvasive
methods to monitor living cells in vitro, the growth of
engineered artificial tissues, and the development of
cell-based biosensors. On all of these matters, Hench
and collaborators successfully integrated Raman
spectroscopy into their studies on tissue regeneration.
They published approximately 25 papers to show the
potential of biophotonic techniques based on Raman
spectroscopy to study biomaterials and cells
[405–427]. Raman spectroscopy is an optical tech-
nique based on inelastic scattering of laser photons
by molecular vibrations, which provides a chemical
fingerprint of biomaterials and cells/organelles
without fixation, lysis or the use of labels, and other
contrast-enhancing chemicals [405–427]. Hench et al.
have employed this technique in situ and in real-time
to follow up HCA formation on biomaterials and
characterize different living and dead cells (e.g.,
osteoblasts, lung cells and stem cells) attached on
them [410, 412]. They elicited Raman signals from
living cells, e.g., for detecting changes in cell pheno-
type, involving irradiating the cell with laser light at
Fig. 8 Biosilicate� prosthesis (Otosilicate) [403].
J Mater Sci
selected wavelengths [427]. They also managed to
show that this spectroscopic method could be used to
study the most important cellular functions involved
in cell–biomaterial interactions, such as cell death,
differentiation, de-differentiation, and mineraliza-
tion. The method offers the potential for studying
cell–bioceramic interactions and reduces the need for
animal testing until the final steps of proving use-
fulness prior to clinical trials [421].
Currently, biophotonics is central to the cancer
studies conducted by Hench’s former students,
Michael Fenn at the Florida Institute of Technology
and Ioan Notingher at the University of Nottingham.
Interested readers can refer to Notingher and Hench’s
highly cited review paper [423] and Fenn et al. [428],
which cover the applications of this technique and
emphasize its potential impact on modern scientific
endeavors, such as tissue engineering, cancer identi-
fication, and drug discovery. They believe that Raman
spectroscopy has the potential not only to improve the
diagnosis of cancer but also to move forward the
treatment of some cancer types [423, 428].
Advanced ceramics (Refs. [429–464])
Thefirst researchproject thatHenchwas involved in as
an engineer intern was related to the chemical vapor
deposition of Al2O3 on UO2 fuel tubes applicable in
nuclear jet engine [35]. Then, as a fresh ceramic engi-
neer, Hench worked at the Lawrence Livermore Lab-
oratory in California to determine the effect of
chemical additives on the sintering of beryllium oxide
(BeO) to be used as the neutron moderator in the
nuclear rocket engine. His first paper on this topic was
presented at the annual meeting of the American
Ceramic Society in 1962 [35]. Then, he worked on sin-
tering and reactions of MgO and Cr2O3 to obtain his
Ph.D degree from Ohio State University in 1964 [429].
At that time, itwasbelieved that anyoxide additive of a
higher or lower valencemetal would enhance the rates
of densification by increasing the concentration of
vacancies, which in turn would enhance diffusion and
sintering. However, the sintering of MgO with the
addition of Cr2O3 was an exception and pressed sam-
ples did not densify. Hench and Russell [429] con-
cluded that when Cr2O3 is heated in air, it reacts with
O2 to form CrO3, which has a high vapor pressure,
evaporates to coat the MgO grains, reacts to form a
spinel (Mg2Cr2O4) that coats the MgO grain
boundaries, and stops diffusion and sintering. Proving
this explanation became Hench’s dissertation [429].
This was the beginning of Hench’s interest in sintering
process and advanced ceramics. Then, he worked on
various aspects of processing and the properties of
Si3N4, Al2O3, and SiC.
Hench and his group performed in-depth work on
sintering and characterization of Si3N4 in the early
1980s, e.g., [439–443]. They utilized Y2O3, MgO, and
ZrO2 additives to improve the sinterability and
properties of Si3N4. Grain boundaries and the role of
the glass phase formation were also investigated by
advanced analysis methods during that time
[439–443]. Wu, Du, Choy, and Hench successfully
densified Al2O3 and TiO2 by laser [451–454]. They
applied powder beds of alumina or titanium dioxide
by aerosol-assisted spray deposition and subse-
quently performed selective laser sintering. Their
studies aimed to understand the effects of laser pro-
cessing parameters on the microstructural evolution
of laser-densified ceramic powder beds and to opti-
mize the laser parameters for laser fabrication
[451–454]. Lee and Hench [446–448] demonstrated
one of the first uses of the sol–gel method to develop
homogenous mixed oxide/non-oxide advanced
composites such as SiC/SiO2, SiC/Al2O3, and SiC/
TiC at low temperatures. Finally, Hench’s book
‘‘Ceramic Processing before Firing’’ has long been
used as a textbook in many countries [26].
Hench and his colleagues also suggested advanced
metallic and ceramic neural stimulating electrodes
[460–464]. They designed appropriate in vitro and
in vivo tests and verified corrosion responses and
physiological/histological properties. These electrodes,
which are implanted in the body, are used to provide
functional neuromuscular control of some organs such
as the bladder, heart, limb, and the respiratory system
[460–464]. For example, they developed electrochemi-
cally anodized tantalum (Ta) capacitive electrodes for
neural stimulation [462]. It was shown through in vitro
studies and preliminary animal experiments that such
electrodes have great promise [462].
Semiconducting and ionic conductingglasses (Refs. [465–485])
Before immersing himself into the realm of bioma-
terials, Hench had his first US Department of Defense
funded project in 1966 as part of a larger
J Mater Sci
multidisciplinary research program on ‘‘Unconven-
tional Semiconductors’’ [35]. He was interested at the
time in investigating the electronic behavior of
vanadium phosphate (V2O5–P2O5) glasses [465, 466].
He demonstrated that these amorphous semicon-
ductors have high electronic conductivity and resist
radiation damage, especially when heat-treated to
induce small ordered regions [467, 468]. This finding
indicated that these new materials might be useable
as electrical switches in satellites, which would need
to survive high doses of high-energy radiation pro-
duced by, e.g., solar flares or certain types of weap-
ons [465–471]. Hench also collaborated in Tehrani’s
Ph.D thesis related to SiC-based semiconductors
[473–477]. Tehrani later became successful and made
a key contribution to the development of magne-
toresistive random access memory (MRAM)
technology.
Hench started a long-time collaboration
(1982–2006) with his Japanese colleague, Yoshihiro
Abe [472, 478–484]. In the early 1980s, the electrical
charge carriers in alkali-free and transition metal-free
oxide glasses were uncertain. Hench and Abe tried to
resolve this ambiguity. They first obtained DC elec-
trical conductivity data for MO�P2O5 glasses
(M = Be, Mg, Ca, Sr, Ba) containing small amounts of
water. Their results suggested that the mobility of
protons (H?) in the glasses increases with decreasing
O–H bonding strength [472]. The relation between
the proton concentration and the conductivity or the
apparent activation energy was studied for calcium
metaphosphate glasses containing various amounts
of water. The conductivity was found to be propor-
tional to the square of the proton concentration [472].
Then, they proved that electrical charge carriers in
lead silicate glasses (with PbO between 30 and
65 mol%) are protons rather than Pb2? by using
quantitative relations between electrical conductivity,
activation energy and the O–H bonding state
[478, 479]. They determined the nature of the elec-
trical charge carriers in oxide glasses containing nei-
ther alkali ions nor transition metal ions, for example,
PbO–SiO2, BaO–SiO2, CaO–SiO2, BaO–P2O5, CaO–
P2O5, glasses. The main charge carrier was protons
(H?) [478–481]. Their fundamental researches finally
led to the development of fast proton-conducting
glassy plates or films having room-temperature con-
ductivities of approximately 10-2 S/cm from the
alkali-free glassy zirconium phosphate synthesized
via sol–gel [482]. The solid amorphous superprotonic
conductors were reported to be chemically stable and
non-hygroscopic in ambient atmosphere even though
they contained molecular water in the structure [482].
The zirconium phosphate gel glasses were suggested
for use as a solid electrolyte in hydrogen cells,
hydrogen gas sensors, and humidity sensors [482].
Finally, they proposed new BaO–La2O3–Al2O3–P2O5
glasses exhibiting high proton conductivities of
10-2 S/cm at 200 �C and 10-3 S/cm at 25 �C with a
low activation energy of 0.17 eV [483]. Figure 9
shows plots of protonic conductivity versus temper-
ature for various compositions of glasses obtained by
Abe et al. [483]. Their findings were useful in devel-
oping H?-conductive glasses as a solid electrolyte
separator in H2–O2 fuel cells. The fuel cell using this
superprotonic glass electrolyte is operable at tem-
peratures from 25 to 200 �C even under non-humid-
ified conditions. To summarize, the protons in oxide
glasses had long been considered to be almost
immobile. However, Hench, Abe and their colleagues
demonstrated that H? is a major charge carrier and
introduced the above cited superprotonic conductors
Figure 9 Protonic conductivity versus 1/T plots for the glasses
obtained by Abe et al. (in ambient atmosphere, Au-electrode, at
10 kHz). Sample 1 22BaO–2.5La2O3–0.5Al2O3–75P2O5 (700 �C).Sample 2 5SrO–15BaO–10PbO–1Al2O3–69P2O5 (600 �C). Sam-
ple 3 6SrO–18BaO–12PbO–64P2O5 (600 �C). Sample 4 12SrO–
12BaO–12PbO–64P2O5 (700 �C). Sample 5 18SrO–6BaO–
12PbO–64P2O5 (800 �C). Glasses (in mole ratio) were prepared
by heating a mixture of raw materials, such as H3PO4 and metal
carbonates, at the listed temperatures for 30 min and subsequently
quenching [483].
J Mater Sci
of phosphate glasses or even modified gypsum
(CaSO4�2H2O) [484] as good candidates for workable
electrolytes of fuel cells.
Glass corrosion and nuclear waste disposal(Refs. [485–545])
In the 1960s, many problems required an under-
standing of glass surface and corrosion. For example,
the stability of glass containers and windows had not
been fully recognized; leaching of nuclear waste
encapsulants was a problem; preservation of glass
antiquities was requested; reliability of fiber optic
interfaces was of great importance; and environ-
mental sensitivity in fracture mechanics was contro-
versial [509]. Therefore, Hench, in his early years at
the University of Florida, together with Sanders,
Person, Clark and Pantano utilized new methods,
e.g., electron microprobe analysis, infrared reflection
spectroscopy, atomic emission spectroscopy, and
Auger spectroscopy, to study glass surface and cor-
rosion [485–498]. Application of these surface analy-
sis instruments was established through a systematic
exploration of a series of glass compositions (mostly
silicate/alkali-silicate glasses) and environments.
Based on their investigations, it became possible to
describe in quantitative detail the surface and bulk
structural state of glassy objects independent of their
processing or environmental history. Characteriza-
tion of glassy objects, e.g., relating composition,
structure, and surface to properties, became possible
because extrinsic processing and environmental
variables could be described in terms of intrinsic
structural features [499–508]. Then, Hench elaborated
on several important glass surface topics that inclu-
ded corrosion mechanisms, the mixed-alkali effect,
surface passivation with solution ions, protective film
formation, the role of CaO, R2O/SiO2, and Al2O3 in
glass corrosion, glass surface area-to-solution volume
ratio, relevance of autoclave procedures in durability
tests, effects of the environment on silica fracture, and
the Bioglass�–bone bonding mechanism [509–529].
These studies provided the fundamental knowledge
that allowed Hench, for example, to propose his well-
known mechanism of bioactivity, which starts with
selective leaching of alkali ions and subsequent silica
gel formation [507].
Hench’s extensive knowledge on glass leaching and
corrosion led to his appointment to coordinate the
Nuclear Regulatory Commission Committee on the
Disposal of Reprocessed High Level Nuclear Wastes.
Hench conducted a number of collaborative research
projects with Belgium, Canada, France, Japan, Swe-
den, Switzerland, the USA, and Germany to test the
relative surface reactions of nuclear waste glasses
(borosilicate glasses) under a wide variety of simu-
lated repository conditions [543]. Nearly 2000 inter-
active interfaces were tested in salt in the Waste
Isolation Pilot Plant site in the United States [531–536].
Other studies included 1-, 3-, 6-, 12-, 24-, and 32-month
deep burial in granite boreholes in the Stripa mine in
Sweden at 90 and 100 �C [537–540]. Several glasses
were also evaluated in limestone for up to 2 years in
the UK [545]. Comparisons of the simulated burial
conditions with glasses containing radioactivity close
to that expected for commercial operations such as
LaHague, France, were made by a Japan–Sweden–
Switzerland consortium with collaboration from the
Commissariat a l’EnergieAtomique,Marcoule and the
Hahn Meitner Institute, Berlin [541–544]. These stud-
ieswere leading toward an international agreement on
the acceptable performance of high-level glassy waste
forms including borosilicate glasses [544]. These
results were challenged by researchers offering crys-
talline materials and concrete waste forms. However,
borosilicate glasswaste forms offered the advantage of
being simpler and demonstrated full-scale and
radioactive remote processing operations [544].
Therefore, Hench’s results and investigations were
supported by the French, who vitrify their nuclear
wastes to this day, and in the USA by PeteMacedo and
his research group at the Catholic University of
America who commercialized a glass encapsulation
program used at several nuclear waste reprocessing
centers, including West Valley, Savannah River and
Hanford [531–545].
Review papers on biomaterials (Refs.[546–582])
Hench wrote more than 30 review papers to elaborate
on his ideas on the history, trends, perspective and
ethical issues of biomaterials and bioceramics. This
valuable collection of papers can be considered a
guide for eventual research and development down a
road that Larry Hench paved for us. We summarize
his flourishing path and inspiring outlooks over the
past 30 years in the following lines.
J Mater Sci
• 1975 Hench improved design criteria and the full
use of bioactive materials. It was apparent to him
that the molecular materials engineering
approach was nearly ready for use in developing
new bioactive biomaterials [546].
• 1979 He recommended that future biomaterials
research and development should focus on
improving reliability and emphasized three areas
of research and development: (1) studies of
composite biomaterials; (2) investigating mecha-
nisms of long-term interfacial reactions; (3) devel-
oping long-term predictive relationships of
biomaterial reliability [547].
• 1980 New composites were developed by Hench
et al. New techniques for characterizing biomate-
rials and their interfaces were also proposed.
These methods became available for predicting
the service lives of materials and prostheses. He
believed that the use of these new materials/
methods should provide better prostheses in the
decade ahead [548].
• 1989 A ‘‘Bioactive Substrate Theory’’ of the origin
of life was elucidated by Hench. The purpose of
the bioactive substrates was considered to activate
the irreversible ordering of macromolecules into
replicative structures. The implications of this
theory on the biochemical design of implants and
the prevention of disease states in modern man
were highlighted by Hench [549].
• 1993 Hench believed that the molecular-based
pharmaceutical approach to the design of bioce-
ramics should couple with the growth of genetic
engineering, sensor technology, and information
processing, resulting in a range of products and
applications not even imagined in the 1980s [551].
• 1996 In his intriguing paper titled ‘‘Life and death:
the ultimate phase transformation’’, he encourages
us to deeply understand the mechanisms under-
lying the mystery of the order (life) $ disorder
(death) transformation similar to glass $ crystal,
which may offer hope for developing new mate-
rials and prolonging the quality of life [555].
• 1999 Hench encouraged the community to have a
vision that synthetic materials may help slow
down, or ideally even reverse, the deterioration
that comes from old age [559].
• 2000 He was expecting to develop a material that
activates the body’s own repair mechanisms,
which is now close to reality. This was a major
shift from replacement of tissues to a new concept
of regeneration of tissues in the new millennium
[561].
• 2005 Assumed that designing a new generation of
gene-activating biomaterials tailored for specific
patients and diseases is possible and feasible.
Now, bioactive stimuli are useful for activating
genes in preventative treatment to maintain the
health of aging tissues [572].
• 2011 Asked for ever more creative and basic
studies on novel glasses and glass–ceramics to
cope with the problems of a world that has finite
resources but infinite desires [577].
• 2015Always believed that there is a great potential
for bioactive ceramics, glasses and glass–ceramics
Figure 10 Sketch of Oscar Peitl’s Ph.D research plan made by
Larry during a discussion with E.D. Zanotto in a bar in Sao Carlos,
SP, Brazil, in 1993. His main goal at that time was to increase the
mechanical properties of Bioglass� 45S5 through controlled
internal crystallization without impairing bioactivity.
J Mater Sci
to achieve a goal of improved healthcare with
reduced costs. In one of his last papers, he could,
fortunately, suggest several major changes in the
field: ‘‘(1) more research and product development
directed toward specific clinical needs of an aging
population, (2) expanded emphasis on areas of
tissue repair other than bone and teeth, and (3)
more concentration on understanding molecular
biology and genetic-based mechanisms of tissue
regeneration and repair’’ [579].
Hench’s editorial note on ‘‘Researchers on research’’
has been a guideline for students and young investi-
gators to start their research work endeavor [580]. He
was an engineer who succeeded in transferring the
results of his basic researches to many candidate
technologies. Then, he and Pennypacker called our
attention to ‘‘making behavioral technology transfer-
able’’ [581]. In their paper, they outlined the process as
it evolved in materials engineering and illustrated its
applicability to behavioral analysis and technology
transfer. They encouraged others to broaden their
efforts in the discipline of behavior analysis in order to
finally fulfill its promise of benefit to the species, as for
sustainable biomaterials and waste disposal tech-
nologies [581]. Finally, ‘‘The bionic Kreidl’’ is a fiction
story written by Hench and Wilson in 1985. However,
many of the applications they envisaged therein were
eventually realized [582].
Concluding remarks
One of us (EDZ) had the fortune of working with
Larry for approximately 20 years. Figure 10 shows
the sketch of Oscar Peitl’s Ph.D research plan made
by Larry in a bar in Sao Carlos, SP, Brazil, in 1993. We
co-authored only two papers [43, 401], one book
chapter [6], and one patent [231], and co-advised the
Ph.D thesis of Oscar Peitl (Federal University of Sao
Carlos, Brazil, and University of Florida, USA).
However, Larry’s legacy on our research group
(www.certev.ufscar.br) was phenomenal: approxi-
mately 30 theses were defended, 44 studies on
bioactive glasses and glass–ceramics were published
[398, 403], 5 patents were registered, and 2 spin-off
companies were born, which collectively received 4
international awards.
Hench was a very clever, knowledgeable, and
enthusiastic person with a charming personality that
fostered collaborations with several hundred stu-
dents and researchers from all of the continents of
this planet. Hench’s success as a teacher/engi-
neer/scientist/colleague is well known. Many of his
students and collaborators are now leading their own
team or are respected professors and researchers in
major universities. We named some of them in this
paper. However, many others have been directly or
indirectly inspired by Hench. Interested readers are
invited to read the great tributes and obituaries that
have been written in his memory [583–585], as the
ones he wrote for David Kingery [586–588].
Prof. Hench not only initiated the field of bioactive
glasses and glass–ceramics but also made several
other important scientific discoveries, such as large
monolithic optical grade silica. It is quite clear that
Larry was one of the most influential materials sci-
entists/engineers of all time! We hope that this
review article is useful as a guide to forthcoming
articles and additionally motivates and encourages
students and younger investigators to dig deeper and
study his prominent publications to design novel
materials and discover new applications. Thank you
Larry for your most useful, enlightening guidance;
the whole ‘‘glass’’ and ‘‘biomaterials’’ communities
will surely miss you!
Acknowledgements
The authors are grateful to the Sao Paulo Research
Foundation—FAPESP, # 2013/07793-6—for the finan-
cial support of this work and for granting a post-
doctoral fellowship to Maziar Montazerian (#
2015/13314-9).
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Bioactive ceramic composition useful in load-bearing
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WO9741079-A; EP896572-A; WO9741079-A1; AU9730
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JP2001526619-W; JP3457680-B2
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DE60204217-E; ES2242851-T3; DE60204225-T2;
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Controlled flocculation of wall tile glaze effluent. Am
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alized aluminosilicate powder for producing structural
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scavenging oil from oil–water mixture, comprises func-
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functionalized surfaces with reactive groups/materials
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fly ash particles useful e.g. for scavenging oil from oil–
water mixture, comprises contacting fly ash particles with
hydroxide compound, and reacting the obtained fly ash
particles with organic alcohol or organic acid,
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treatment on electrical properties of a K2PO3–V2O5 semi-
conducting glass. Am Ceram Soc Bull 47(4):398
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Observation of single-carrier space-charge-limited flow in
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conduction in oxide glasses—simple relations between
electrical-conductivity, activation-energy, and the O–H
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(1991) Evidence for protonic conduction in alkali-free
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Superprotonic conductors of glassy zirconium phosphates.
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Conversion of gypsum into a superprotonic conductor.
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[485] Hench LL (1969) Humidity effects in electronic substrates.
Am Ceram Soc Bull 48(8):803
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[487] Clark DE, Hench LL (1972) Sample preparation variables
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[496] Sanders DM, Hench LL (1973) Environmental effects on
glass corrosion kinetics. Am Ceram Soc Bull 52(9):662
[497] Hench LL, Sanders DM, Dilmore MF, Ethridge EC (1973)
Structural-analysis of corrosion processes of commercial
glasses. Am Ceram Soc Bull 52(4):380
[498] Clark AE, Hench LL (1973) Effect of P5?, B3? and F-
additions on corrosion of Na2O–CaO–SiO2 glasses. Am
Ceram Soc Bull 52(4):379
[499] Sanders DM, Person WB, Hench LL (1974) Quantitative-
analysis of glass structure with use of infrared reflection
spectra. Appl Spectrosc 28(3):247–255
[500] Ethridge EC, Hench LL (1974) Effects of compositional
range on alkali-silicate glass corrosion kinetics. Am Ceram
Soc Bull 53(4):349
[501] Dilmore MF, Hench LL (1974) Corrosion behavior of
Li2O–Al2O3–SiO2 glasses. Am Ceram Soc Bull 53(4):349
[502] Clark DE, Hench LL, Acree WA (1975) Electron-micro-
probe analysis of Na2O–CaO–SiO2 glass. J Am Ceram Soc
58(11–1):531–532
[503] Gokularathnam CV, Gould RW, Hench LL (1975) Effect of
water on structure of vitreous silica. Phys Chem Glasses
16(1):13–16
[504] Hench LL (1975) Characterization of glass corrosion and
durability. J Non Cryst Solids 19:27–39
[505] Clark DE, Acree WA, Hench LL (1976) Electron-micro-
probe analysis of corroded soda-lime-silica glasses. J Am
Ceram Soc 59(9–10):463–464
[506] Clark DE, Dilmore MF, Ethridge EC, Hench LL (1976)
Aqueous corrosion of soda-silica and soda-lime-silica glass.
J Am Ceram Soc 59(1–2):62–65
[507] Clark AE, Pantano CG, Hench LL (1976) Auger spectro-
scopic analysis of Bioglass corrosion films. J Am Ceram
Soc 59(1–2):37–39
[508] Pantano CG, Hench LL (1977) Cleaning borosilicate glass
for biological application. J Test Eval 5(1):66–69
[509] Hench LL (1977) Physical-chemistry of glass surfaces.
J Non Cryst Solids 25(1–3):343–369
[510] Clark DE, Ethridge EC, Dilmore MF, Hench LL (1977)
Quantitative-analysis of corroded glass using infrared fre-
quency-shifts. Glass Technol 18(4):121–124
[511] Ethridge EC, Hench LL (1977) Static corrosion of glass.
Am Ceram Soc Bull 56(3):330
[512] Ethridge EC, Hench LL (1977) Mechanisms of glass cor-
rosion. Am Ceram Soc Bull 56(3):330
[513] Dilmore MF, Hench LL (1977) Role of aluminum ions in
glass durability. Am Ceram Soc Bull 56(3):330
[514] Dilmore MF, Hench LL (1977) Role of mixed-alkali effect
on glass durability. Am Ceram Soc Bull 56(3):330
[515] Dilmore MF, Clark DE, Hench LL (1978) Chemical dura-
bility of Na2O–K2O–CaO–SiO2 glasses. J Am Ceram Soc
61(9–10):439–443
[516] Hench LL, Clark DE (1978) Physical-chemistry of glass
surfaces. J Non Cryst Solids 28(1):83–105
[517] Dilmore MF, Clark DE, Hench LL (1978) Aqueous cor-
rosion of lithia-alumina-silicate glasses. Am Ceram Soc
Bull 57(11):1040–1044
[518] Palmer RA, Hench LL (1979) Nondestructive evaluation of
surface flaws using infrared reflection spectroscopy. Am
Ceram Soc Bull 58(3):384
[519] Ethridge EC, Clark DE, Hench LL (1979) Effects of glass-
surface area to solution volume ratio on glass corrosion.
Phys Chem Glasses 20(2):35–40
[520] Hench LL, Newton RG, Bernstein S (1979) Use of infrared
reflection spectroscopy in analysis of durability of medieval
glasses, with some comments on conservation procedures.
Glass Technol 20(4):144–148
[521] Dilmore MF, Clark DE, Hench LL (1979) Corrosion
behavior of lithia disilicate glass in aqueous-solutions of
aluminum compounds. Am Ceram Soc Bull 58(11):1111
[522] Mccracken WJ, Clark DE, Hench LL (1979) Effects of
solution pH on corrosion behavior of Li2O�2SiO2 glass-
ceramics. Am Ceram Soc Bull 58(3):382
[523] Clark DE, Yenbower EL, Hench LL (1979) Corrosion
behavior of a zinc-borosilicate simulated nuclear waste
glass. Am Ceram Soc Bull 58(3):324
[524] Hench LL (1980) Control of glass surfaces. Am Ceram Soc
Bull 59(8):864
[525] Chao Y, Clark D, Hench LL (1980) Weathering of Na2-O�2SiO2 glass. Am Ceram Soc Bull 59(8):864
[526] Hench LL (1982) Glass surfaces—1982. J Phys 43(NC-
9):625–636
[527] Hench LL, Clark DE (1982) Surface-analysis of glasses. CS
symposium series, vol 199, pp 203–229
[528] Bendale RD, Hench LL (1995) Molecular-orbital models of
strained tetrahedral edge shared active-sites on dehydrox-
ylated silica—an AM1 and PM3 study. Surf Sci
338(1–3):322–328
[529] West JK, Hench LL (1998) The effect of environment on
silica fracture: vacuum, carbon monoxide, water and
nitrogen. Philos Mag A Phys Condens Matter Struct
Defects Mech Prop 77(1):85–113
[530] Hench LL, Smith D, Cason B, Housefie LG (1973) Con-
trolled flocculation of tile glaze wastes. Am Ceram Soc Bull
52(4):418
[531] Hench LL, Clark DE, Yenbower EL (1979) Approach to
long-term prediction of stability of nuclear waste forms.
Am Ceram Soc Bull 58(3):319
J Mater Sci
[532] Hench LL (1980) Waste forms—methods of predicting
long-term performance of glasses and other alternatives.
Bull Am Phys Soc 25(4):499
[533] Hench AA, Hench LL (1983) Computer-analysis of nuclear
waste glass composition effects on leaching. Nucl Chem
Waste Manag 4(3):231–238
[534] Werme LO, Hench LL, Nogues JL, Odelius H, Lodding A
(1983) On the pH-dependence of leaching of nuclear waste
glasses. J Nucl Mater 116(1):69–77
[535] Hench LL, Clark DE, Campbell J (1984) High-level waste
immobilization forms. Nucl Chem Waste Manag
5(2):149–173
[536] Hench LL, Spilman DB, Buonaquisti AD (1984) Ruther-
ford back scattering surface-analysis of nuclear waste
glasses after one year burial in Stripa. Nucl Chem Waste
Manag 5(1):75–85
[537] Lodding A, Hench LL, Werme L (1984) Nuclear waste
glass interfaces after one year burial in Stripa. 2. Glass
bentonite. J Nucl Mater 125(3):280–286
[538] Hench LL, Lodding A, Werme L (1984) Nuclear waste
glass interfaces after one year burial in Stripa. 1. Glass
glass. J Nucl Mater 125(3):273–279
[539] Hench LL, Werme L, Lodding A (1984) Nuclear waste
glass interfaces after one year burial in Stripa. 3. Glass
granite. J Nucl Mater 126(3):226–233
[540] Hench LL, Wilson MJR (1985) Nuclear waste glass inter-
faces after one year burial in Stripa. 4. Comparative surface
profiles. J Nucl Mater 136(2–3):218–228
[541] Maurer C, Clark DE, Hench LL, Grambow B (1985) Sol-
ubility effects on the corrosion of nuclear defense waste
glasses. Nucl Chem Waste Manag 5(3):193–201
[542] Zhu BF, Clark DE, Hench LL, Wicks GG (1986) Leaching
behavior of nuclear waste glass heterogeneities. J Non
Cryst Solids 80(1–3):324–334
[543] Hench LL (1986) International collaboration in nuclear
waste solidification. Nucl Technol 73(2):188–198
[544] Hench LL, Clark DE, Harker AB (1986) Nuclear waste
solids. J Mater Sci 21(5):1457–1478. doi:10.1007/
BF01114698
[545] Namboodri CG; Namboodri SL; Wicks GG; Lodding AR;
Hench LL; Clark DE; Newton RG; Surface-analyses of
SRS waste glass buried for up to 2 years in limestone in the
united-kingdom. In: Wicks GG; Bickford DF; Bunnell LR
(eds) 5th international symposium at the 93rd annual
meeting of the American Ceramic Society: ceramics in
nuclear and hazardous waste management, Cincinnati, OH,
28 Apr–02 May 1991, nuclear waste management IV.
Ceramic transactions, vol 23, pp 653–662
[546] Hench LL (1975) Prosthetic implant materials. Annu Rev
Mater Sci 5:279–300
[547] Hench LL (1979) Future-developments and applications of
biomaterials—overview. Biomater Med Devices Artif
Organs 7(2):339–350
[548] Hench LL (1980) Biomaterials. Science
208(4446):826–831
[549] Hench LL (1989) Bioceramics and the origin of life.
J Biomed Mater Res 23(7):685–703
[550] Hench LL, Wilson J (1991) Bioceramics. MRS Bull
16(9):62–74
[551] Hench LL (1993) Bioceramics—from concept to clinic.
Am Ceram Soc Bull 72(4):93–98
[552] Hench LL (1994) Bioactive ceramics: theory and clinical
applications. In: Andersson OH, Happonen RP, YliUrpo A
(eds) 7th international symposium on ceramics in medicine,
Turku, Finland, 28–30 July 1994, bioceramics, vol 7,
pp 3–14
[553] Hench LL (1995) Inorganic biomaterials. In: Interrante LV,
Caspar LA, Ellis AB (eds) Symposium on materials
chemistry—an emerging discipline, at the 204th National
Meeting of the American-Chemical-Society, Washington,
DC, 23–28 Aug 1992, materials chemistry: an emerging
discipline. Advances in chemistry series, vol 245,
pp 523–547
[554] Hench LL (1995) Bioactive implants. Chem Ind
14:547–550
[555] Hench LL (1996) Life and death: the ultimate phase
transformation. Thermochim Acta 280:1–13
[556] Hench LL (1997) Introduction to biomaterials. Anales
Quim 93(1):S3–S5
[557] Hench LL (1998) Bioceramics, a clinical success. Am
Ceram Soc Bull 77(7):67–74
[558] Hench LL (1999) Role of inorganic and theoretical chem-
istry in ceramics: past, present, and future. Br Ceram Trans
98(5):246–250
[559] Hench LL (1999) Medical materials for the next millen-
nium. MRS Bull 24(5):13–19
[560] Ratner BD, Hench LL (1999) Perspectives on biomaterials.
Curr Opin Solid State Mater Sci 4(4):379–380
[561] Hench LL (2000) The challenge of orthopaedic materials.
Curr Orthop 14(1):7–15
[562] Hench LL (2000) A genetic theory of bioactive materials.
In: Giannini S, Moroni A (eds) 13th international sympo-
sium on ceramic in medicine/symposium on ceramic
materials in orthopaedic surgery: clinical results in the year
2000, Bologna, Italy, 22–26 Nov 2000, bioceramics. Key
engineering materials, vol 192, no 1, pp 575–580
[563] Hench LL, Polak JM, Xynos ID, Buttery LDK (2000)
Bioactive materials to control cell cycle. Mater Res Inno-
vations 3(6):313–323
J Mater Sci
[564] Jones JR, Hench LL (2001) Materials perspective—
Biomedical materials for new millennium: perspective on
the future. Mater Sci Technol 17(8):891–900
[565] Hench LL, Xynos ID, Edgar AJ, Buttery LDK, Polak JM
(2002) A genetic basis for biomedical materials. In:
McLean M (eds) Conference on materials science and
engineering, Imperial College Science, Technology and
Medicine, London, England, 14–15 May 2001, materials
science and engineering: its nucleation and growth,
pp 283–296
[566] Hench LL (2002) Ceramic engineering design: designing a
bionic cat. In: Clark DE, Folz DC, McGee TD (eds)
Workshop on designing with engineering ceramics, Cocoa
Beach, FL, Jan 2001. Introduction to ceramic engineering
design, pp 374–391
[567] Cleevely ST, Hench L (2002) Professor Larry Hench—
making discoveries in the biomaterials field. Mater World
10(11):12
[568] Hench LL, Boccaccini AR, Day RM et al (2003) Third-
generation gene-activating biomaterials. In: Chandra T,
Torralba JM, Sakai T (eds) 4th international conference on
processing and manufacturing of advanced materials, Univ.
Carlos III Madrid, Madrid, Spain, 07–11 Jul 2003, Ther-
mec’2003, PTS 1–5. Materials science forum, vol 426, no
4, pp 179–184
[569] Hench LL (2003) The role of ceramics in an age of biology.
In: Sundar V, Rusin RP, Rutiser CA (eds) Symposium on
bioceramics held at the 105th annual meeting of the
American-Ceramic-Society, Nashville, TN, 27–30 Apr
2003 bioceramics: materials and applications IV. Ceramic
transactions, vol 147, pp 3–12
[570] Hench LL (2003) Glass and genes: the 2001 W. E. S. turner
memorial lecture. Glass Technol 44(1):1–10
[571] Shirtliff VJ, Hench LL (2003) Bioactive materials for tissue
engineering, regeneration and repair. J Mater Sci
38(23):4697–4707. doi:10.1023/A:1027414700111
[572] Hench LL (2005) Challenges for bioceramics in the 21st
century. Am Ceram Soc Bull 84(9):18–21
[573] Polak J, Hench L (2005) Gene therapy progress and pro-
spects: in tissue engineering. Gene Ther 12(24):1725–1733
[574] Karakoti AS, Hench LL, Seal S (2006) The potential toxicity
of nanomaterials—the role of surfaces. JOM 58(7):77–82
[575] Maroothynaden J, Hench LL (2006) The effect of micro-
gravity and bioactive surfaces on the mineralization of
bone. JOM 58(7):57–63
[576] Hench LL, Thompson I (2010) Twenty-first century chal-
lenges for biomaterials. J R Soc Interface 7(4):S379–S391
[577] Hench LL (2011) Glass and glass-ceramic technologies to
transform the world. Int J Appl Glass Sci 2(3):162–176
[578] Hench LL (2014) Bio-ceramics for the next 25 years:
challenges and opportunities. In: Antoniac I, Cavalu S,
Traistaru T (eds) 25th symposium and annual meeting of
the international-society-for-ceramics-in-medicine (ISCM),
Bucharest, Romania, 07–10 Nov 2013 bioceramics, vol 25.
Key engineering materials, vol 587, pp 3–14
[579] Hench LL (2015) The future of bioactive ceramics. J Mater
Sci Mater Med 26(2):86
[580] Hench L, Mote D, Sorenson S, Martin R (1973)
Researchers on research. Eng Educ 63(4):268–272
[581] Pennypacker HS, Hench LL (1997) Making behavioural
technology transferable. Behav Anal 20(2):97–108
[582] Hench L, Wilson J (1985) The bionic kreidl. J Non Cryst
Solids 73(1–3):R13–R16
[583] Simmons JH (2016) The professional life of Larry L.
Hench—a true renaissance scientist/engineer. J Non Cryst
Solids: JNCS 436:58–61
[584] Bonfield W (2006) A tribute to Professor Larry Hench.
J Mater Sci Mater Med 17(11):965–966
[585] Schoen HJ, Greenspan DC (2016) In memoriam Larry L.
Hench, Ph.D. 1938–2015. J Biomed Mater Res Part A
104(4):819–820
[586] Hench LL (1967) His heart in ceramics. Am Ceram Soc
Bull 46(5):A10
[587] Hench LL, Uhlmann DR (2000) Obituary—Professor W.D.
Kingery. Ceram Int 26(8):797–799
[588] Hench LL, Uhlmann DR (2000) W. David Kingery—
obituary. Ind Ceram 20(2):131
J Mater Sci