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

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.6b02878· OSTI ID:1466697
 [1];  [1];  [1];  [2];  [1];  [2];  [3];  [2];  [1];  [1];  [4];  [2]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Chinese Academy of Sciences, Shanxi (China); Synfuels China, Beijing (China)
  4. 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.

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
Citation Metrics:
Cited by: 269 works
Citation information provided by
Web of Science

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Reduced SnO 2 Porous Nanowires with a High Density of Grain Boundaries as Catalysts for Efficient Electrochemical CO 2 -into-HCOOH Conversion journal February 2017
Two‐Dimensional Electrocatalysts for Efficient Reduction of Carbon Dioxide journal October 2019
Understanding the role of functional groups of thiolate ligands in electrochemical CO 2 reduction over Au(111) from first-principles journal January 2019
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Chelating N-Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO 2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry journal March 2018
Ligand-regulated ORR activity of Au nanoparticles in alkaline medium: the importance of surface coverage of ligands journal January 2018
N‐Heterocyclic Carbene‐Modified Au–Pd Alloy Nanoparticles and Their Application as Biomimetic and Heterogeneous Catalysts journal November 2018
Cyclopentadienone iron complexes as efficient and selective catalysts for the electroreduction of CO 2 to CO journal January 2017
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Abundant Ce 3+ Ions in Au‐CeO x Nanosheets to Enhance CO 2 Electroreduction Performance journal April 2019
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Progress in development of electrocatalyst for CO 2 conversion to selective CO production journal March 2020
Current achievements and the future direction of electrochemical CO 2 reduction: A short review journal June 2019
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