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Title: Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides

Abstract

Electrochemical CO 2 reduction reaction (CO 2RR) with renewable electricity is a potentially sustainable method to reduce CO 2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO 2RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO 2RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO 2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. As a result, this work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO 2RR activity.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [2]
  1. Tianjin Univ., Tianjin (People's Republic of China); Columbia Univ., New York, NY (United States)
  2. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Columbia Univ., New York, NY (United States)
  4. Tianjin Univ., Tianjin (People's Republic of China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1542779
Alternate Identifier(s):
OSTI ID: 1504298
Report Number(s):
BNL-211861-2019-JAAM
Journal ID: ISSN 0044-8249
Grant/Contract Number:  
SC0012704; FG02-13ER16381; SC0009476
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Volume: 131; Journal Issue: 19; Journal ID: ISSN 0044-8249
Publisher:
German Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CO2 electroreduction; carbides; in-situ X-ray spectroscopy; computational chemistry; palladium hydride

Citation Formats

Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, and Chen, Jingguang G. Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides. United States: N. p., 2019. Web. doi:10.1002/ange.201900781.
Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, & Chen, Jingguang G. Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides. United States. doi:10.1002/ange.201900781.
Wang, Jiajun, Kattel, Shyam, Hawxhurst, Christopher J., Lee, Ji Hoon, Tackett, Brian M., Chang, Kuan, Rui, Ning, Liu, Chang ‐Jun, and Chen, Jingguang G. Mon . "Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides". United States. doi:10.1002/ange.201900781.
@article{osti_1542779,
title = {Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO2 by Supporting Palladium on Metal Carbides},
author = {Wang, Jiajun and Kattel, Shyam and Hawxhurst, Christopher J. and Lee, Ji Hoon and Tackett, Brian M. and Chang, Kuan and Rui, Ning and Liu, Chang ‐Jun and Chen, Jingguang G.},
abstractNote = {Electrochemical CO2 reduction reaction (CO2RR) with renewable electricity is a potentially sustainable method to reduce CO2 emissions. Palladium supported on cost-effective transition-metal carbides (TMCs) are studied to reduce the Pd usage and tune the activity and selectivity of the CO2RR to produce synthesis gas, using a combined approach of studying thin films and practical powder catalysts, in situ characterization, and density functional theory (DFT) calculations. Notably, Pd/TaC exhibits higher CO2RR activity, stability and CO Faradaic efficiency than those of commercial Pd/C while significantly reducing the Pd loading. In situ measurements confirm the transformation of Pd into hydride (PdH) under the CO2RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. As a result, this work suggests the prospect of using TMCs as low-cost and stable substrates to support and modify Pd for enhanced CO2RR activity.},
doi = {10.1002/ange.201900781},
journal = {Angewandte Chemie},
number = 19,
volume = 131,
place = {United States},
year = {2019},
month = {3}
}

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This content will become publicly available on March 18, 2020
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