A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1466697
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 138; Journal Issue: 26; Related Information: © 2016 American Chemical Society.; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Cao, Zhi, Kim, Dohyung, Hong, Dachao, Yu, Yi, Xu, Jun, Lin, Song, Wen, Xiaodong, Nichols, Eva M., Jeong, Keunhong, Reimer, Jeffrey A., Yang, Peidong, and Chang, Christopher J.. A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b02878.
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.. A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction. United States. https://doi.org/10.1021/jacs.6b02878
Cao, Zhi, Kim, Dohyung, Hong, Dachao, Yu, Yi, Xu, Jun, Lin, Song, Wen, Xiaodong, Nichols, Eva M., Jeong, Keunhong, Reimer, Jeffrey A., Yang, Peidong, and Chang, Christopher J.. Mon .
"A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction". United States. https://doi.org/10.1021/jacs.6b02878. https://www.osti.gov/servlets/purl/1466697.
@article{osti_1466697,
title = {A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction},
author = {Cao, Zhi and Kim, Dohyung and Hong, Dachao and Yu, Yi and Xu, Jun and Lin, Song and Wen, Xiaodong and Nichols, Eva M. and Jeong, Keunhong and Reimer, Jeffrey A. and Yang, Peidong and Chang, Christopher J.},
abstractNote = {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.},
doi = {10.1021/jacs.6b02878},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 138,
place = {United States},
year = {2016},
month = {6}
}
Web of Science
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Highly Efficient CO 2 Electroreduction on ZnN 4 -based Single-Atom Catalyst
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Systematically Tuning the Electronic Structure of Gold Nanoclusters through Ligand Derivatization
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Recent Advances in the Chemistry of N ‐Heterocyclic‐Carbene‐Functionalized Metal‐Nanoparticles and Their Applications
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Robust gold nanorods stabilized by bidentate N-heterocyclic-carbene–thiolate ligands
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Progress in catalyst exploration for heterogeneous CO 2 reduction and utilization: a critical review
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Ultrasmall Au nanocatalysts supported on nitrided carbon for electrocatalytic CO 2 reduction: the role of the carbon support in high selectivity
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Oxygen vacancy associated single-electron transfer for photofixation of CO2 to long-chain chemicals
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Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO 2
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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
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Selective Electrochemical Reduction of Carbon Dioxide to Ethanol on a Boron- and Nitrogen-Co-doped Nanodiamond
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Nanocrystal/Metal–Organic Framework Hybrids as Electrocatalytic Platforms for CO 2 Conversion
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A Polymer Solution To Prevent Nanoclustering and Improve the Selectivity of Metal Nanoparticles for Electrocatalytic CO 2 Reduction
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A Benchtop Method for Appending Protic Functional Groups to N‐Heterocyclic Carbene Protected Gold Nanoparticles
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Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO 2 Reduction
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Systematically Tuning the Electronic Structure of Gold Nanoclusters through Ligand Derivatization
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An N-heterocyclic carbene ligand promotes highly selective alkyne semihydrogenation with copper nanoparticles supported on passivated silica
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Progress and Perspective of Electrocatalytic CO 2 Reduction for Renewable Carbonaceous Fuels and Chemicals
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Host–Guest Chemistry Meets Electrocatalysis: Cucurbit[6]uril on a Au Surface as a Hybrid System in CO2 Reduction
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Citrate-Capped Hybrid Au-TiO2 Nanomaterial for Facile and Enhanced Electrochemical Hydrazine Oxidation
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Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis
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Bismuthene for highly efficient carbon dioxide electroreduction reaction
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Review on optofluidic microreactors for artificial photosynthesis
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