A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

Cao, Zhi; Kim, Dohyung; Hong, Dachao; Yu, Yi; Xu, Jun; Lin, Song; Wen, Xiaodong; Nichols, Eva M.; Jeong, Keunhong; Reimer, Jeffrey A.; Yang, Peidong; Chang, Christopher J.

doi:10.1021/jacs.6b02878

Title: A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

Journal Article · 20 June 2016 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.6b02878 · OSTI ID:1466697

Cao, Zhi ^[1]; Kim, Dohyung ^[1]; Hong, Dachao ^[1]; Yu, Yi ^[2]; Xu, Jun ^[1]; Lin, Song ^[2]; Wen, Xiaodong ^[3]; Nichols, Eva M. ^[2]; Jeong, Keunhong ^[1]; Reimer, Jeffrey A. ^[1]; Yang, Peidong ^[4]; Chang, Christopher J. ^[2]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Chinese Academy of Sciences, Shanxi (China); Synfuels China, Beijing (China)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy Nanosciences Institute, Berkeley, CA (United States)

Conversion of the greenhouse gas carbon dioxide (CO₂) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO₂ to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO₂ to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO₂ reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1466697

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 26; Related Information: © 2016 American Chemical Society.; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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