Supporting Information

Multilayered Polyion Complexes with Dissolvable Silica Layer

Covered by Controlling Densities of cRGD-conjugated PEG Chains for

Cancer-targeted siRNA Delivery

Mitsuru Naitoa, Ryota Azumab, Hiroyasu Takemotoc, Mao Horid, Naoto

Yoshinagad, Shigehito Osawae, Rimpei Kamegawab, Hyun Jin Kima,

Takehiko Ishiid, Nobuhiro Nishiyamac, Kanjiro Miyataa,b*, Kazunori

Kataokae,f**

aCenter for Disease Biology and Integrative Medicine, Graduate School of Medicine,

The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan

bDepartment of Materials Engineering, Graduate School of Engineering, The University

of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

cLaboratory for Chemistry and Life Science, Institute of Innovative Research, Tokyo

Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan

dDepartment of Bioengineering, Graduate School of Engineering, The University of

Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

eInnovation Center of NanoMedicine, Institute of Industry Promotion-KAWASAKI, 3-

25-14 Tonomachi, Kawasaki-ku, Kawasaki 210-0821, Japan

fPolicy Alternatives Research Institute, The University of Tokyo, 7-3-1 Hongo, Bunkyo-

ku, Tokyo 113-0033, Japan

Corresponding author.

*Email: miyata@bmw.t.u-tokyo.ac.jp

**Email: kataoka@pari.u-tokyo.ac.jp

1

Scheme S1. Synthesis scheme of cRGD-PEG-PAsp(TEP).

2

Figure S1. 1H NMR spectrum of PAsp(TEP) (polymer concentration: 10 mg/mL,

solvent: D2O, temperature: 80 °C).

3

Figure S2. 1H NMR spectrum of cRGD-PEG-PAsp(TEP) (polymer concentration: 10

mg/mL, solvent: D2O, temperature: 80 °C).

4

Figure S3. (a) Cumulant diameter and PDI of template PICs prepared at varying N/P

ratios. (b) Cumulant diameter and PDI of sPICs prepared at varying concentrations of

sodium silicate. (c) Cumulant diameter of mPICs prepared at varying concentrations of

cRGD-PEG-PAsp(TEP).

Figure S4. TEM images of (a) template PIC, (b) sPIC-7.5, (c) sPIC-10, and (d) sPIC-15

(Scale bar: 200 nm).

5

Figure S5. STEM-EDS image of sPIC-15. Cross marks indicate the points where atomic

mass ratios were analyzed (Scale bar: 100 nm).

Figure S6. Intensity-weighted size distribution histograms of a series of mPICs

measured by DLS.

6

Figure S7. (a) Agarose gel retardation analysis of a series of PICs. (b) Encapsulation

efficiency of siRNA in each PIC sample, determined by densitometry of the gel.

Figure S8. Viability of cultured HeLa-Luc cells after 48 h incubation with (+)mPICs

with siCon (siRNA concentration: 100 nM). The cell viabilities were determined using

CCK-8. Results are expressed as mean ± SD (n = 5).

7