Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction

Gong, Ming; Cao, Zhi; Liu, Wei; Nichols, Eva M.; Smith, Peter T.; Derrick, Jeffrey S.; Liu, Yi-Sheng; Liu, Jinjia; Wen, Xiaodong; Chang, Christopher J.

doi:10.1021/acscentsci.7b00316

Title: Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction

Journal Article · Wed Sep 13 00:00:00 EDT 2017 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.7b00316· OSTI ID:1389889

Gong, Ming; Cao, Zhi; Liu, Wei; Nichols, Eva M.; Smith, Peter T.; Derrick, Jeffrey S.; Liu, Yi-Sheng; Liu, Jinjia ^[1];

^[2];

Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001, China
Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001, China, Synfuels China, Beijing, 100195, China

Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO₂) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here in this paper, we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm²) at a potential of -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: 101528-002; AC02-05CH11231

OSTI ID:: 1389889

Alternate ID(s):: OSTI ID: 1416929

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Vol. 3 Journal Issue: 9; ISSN 2374-7943

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 47 works

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