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OBJECTIVEINTRODUCTION

Design and Synthesis of Electrochemically Active Metal Organic Frameworks for Voltage-Driven Capture and Release of Ethylene

Ethylene is widely used within the chemical industry, and isproduced more than any other organic compound.Currently, the purification process of ethylene (e.g. steamor catalytic cracking and cryogenic distillation) is energy-intensive and expensive. Wang and Steifel proposed thatthe use of voltage-driven, chemically specific separationreagents, such as nickel-dithiolene complex, can be apotentially inexpensive and efficient approach for thepurification of olefins.

EXPERIMENTAL DESIGN

Metal Organic Frameworks (MOFs) have remarkableproperties that may help address global challenges in gaspurification. The design and synthesis of MOFs that can actas nanostructured porous electrodes to enable reversiblebinding of ethylene may advance energy-efficient strategiesfor the purification and separation of olefins.

Synthesis of HTTP:

Special thanks to the Mirica Group, the Women in Science Program, and the Dartmouth Chemistry Department.

V

Multicomponent

Stream (MCS)

+

MCS

V2

V1

MOF

electrochemically active

porous solid supported

MOF nanostructures

voltage-actuated

capture and release

of ethylene

ligand

MCS without

purified

(a) R. Eisenberg et al., Inorg. Chem., 2011, 50, 9741-9751. (b) K. Wang et al., Science, 2001, 291 106-108

Here we illustrate the theory behind purification of ethyleneby Ni-bisdithiolene based MOFs. Increasing the size of thebisdithiolene-containing aromatic backbone increases theporosity and the electron density, affecting the efficiency ofethylene capture and purification.

dd d

L1

L2

L3

Hypothesis 1: increasing diameter (affects gas diffusion kinetics)

Hypothesis 2: decreasing band gap (affects activation energy, conductivity, electrochemistry)

L1: Kambe et al., J. Am. Chem. Soc., 2013, 135. Liu et al., J. Phys. Chem., 2016, 120.L2: Marinescu et al., J. Am. Chem. Soc., 2015, 137. Cui and Xu, Chem. Commun., 2014, 50, 3986. Dong et al., Angew. Chem. Int. Ed., 2015, 54.

0

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1600

0 1 2 3 4 5 6 7 8 9 10

Co

un

ts

Energy (keV)

EDS of Cu3(HTTP)2 MOF on HOPG

Cu

C

Cu

CuO

S

Cu

Cu3(HTTP)2 MOF:

Ni3(HTTP)2 MOF:

Co3(HTTP)2 MOF:R. Dong et al., Angew. Chem. Int. Ed., 2015, 54.

Synthesis of MOF:

Alice Hsu, WISP Intern; Xiaoping Zhang, Post-Doc; Katherine Mirica, PI; Mirica Group. Affiliation: Department of Chemistry, Dartmouth College

M I R I C AG R O U P

2μm 1μm10μm

10μm 2μm20μm

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Co

un

ts

Energy (keV)

EDS of Ni3(HTTP)2MOF on HOPG

C

O

Ni

Si

S

SNi

Ni

2μm 2μm5μm

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7000

0 1 2 3 4 5 6 7 8 9 10

Co

un

ts

Energy (keV)

EDS of Co3(HTTP)2 MOF on HOPGC

O

Co Si

SCo Co

Co

METHODS

ACKNOWLEDGEMENTS

• HTTP has been successfully made and characterized.

• MOFs form nanocrystals on HOPG surface differentlydepending on the metal center.

• Continue the synthesis and characterization of HTTP-based MOFs with different metal centers.

M I R I C AG R O U P

RESULTS

CONCLUSIONS AND FUTURE WORK

A B C

D E F

G H I