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Title: Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane

Abstract

Developing sustainable energy strategies based on CO 2 reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO 2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO 2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO 2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO 2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO 2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO 2 resulting in the enhancement of catalytic current densities by threefold. In conclusion, the procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1]
  1. Univ. of North Carolina at Chapel Hill, Chapel Hill, NC (United States)
  2. Univ. of the West Indies, Kingston (Jamaica)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for Solar Fuels (UNC EFRC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1235505
Alternate Identifier(s):
OSTI ID: 1370858
Grant/Contract Number:  
SC0001011
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 112; Journal Issue: 52; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); hydrogen and fuel cells; electrodes - solar; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); solar energy; carbon dioxide reduction; CuPd nanoalloy; electropolymerized film; hydrocarbon

Citation Formats

Zhang, Sheng, Kang, Peng, Bakir, Mohammed, Lapides, Alexander M., Dares, Christopher J., and Meyer, Thomas J. Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane. United States: N. p., 2015. Web. doi:10.1073/pnas.1522496112.
Zhang, Sheng, Kang, Peng, Bakir, Mohammed, Lapides, Alexander M., Dares, Christopher J., & Meyer, Thomas J. Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane. United States. doi:10.1073/pnas.1522496112.
Zhang, Sheng, Kang, Peng, Bakir, Mohammed, Lapides, Alexander M., Dares, Christopher J., and Meyer, Thomas J. Mon . "Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane". United States. doi:10.1073/pnas.1522496112.
@article{osti_1235505,
title = {Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane},
author = {Zhang, Sheng and Kang, Peng and Bakir, Mohammed and Lapides, Alexander M. and Dares, Christopher J. and Meyer, Thomas J.},
abstractNote = {Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. In conclusion, the procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.},
doi = {10.1073/pnas.1522496112},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 52,
volume = 112,
place = {United States},
year = {2015},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1522496112

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Cited by: 24 works
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    Works referencing / citing this record:

    Cobalt Complex with Redox-Active Imino Bipyridyl Ligand for Electrocatalytic Reduction of Carbon Dioxide to Formate
    journal, May 2018