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

Abstract

Abstract Electrochemical CO 2 reduction reaction (CO 2 RR) 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 2 RR 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 2 RR 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 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low‐cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [2]
  1. Collaborative Innovation Center of Chemical Science and Engineering School of Chemical Engineering and Technology Tianjin University Tianjin 300072 P. R. China, Department of Chemical Engineering Columbia University 500 W. 120th St. New York NY 10027 USA
  2. Department of Chemical Engineering Columbia University 500 W. 120th St. New York NY 10027 USA, Chemistry Department Brookhaven National Laboratory Upton NY 11973 USA
  3. Department of Chemical Engineering Columbia University 500 W. 120th St. New York NY 10027 USA
  4. Collaborative Innovation Center of Chemical Science and Engineering School of Chemical Engineering and Technology Tianjin University Tianjin 300072 P. R. China
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1504498
Grant/Contract Number:  
FG02-13ER16381; SC0009476
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition) Journal Volume: 58 Journal Issue: 19; Journal ID: ISSN 1433-7851
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

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 CO 2 by Supporting Palladium on Metal Carbides. Germany: N. p., 2019. Web. doi:10.1002/anie.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 CO 2 by Supporting Palladium on Metal Carbides. Germany. https://doi.org/10.1002/anie.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. 2019. "Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 by Supporting Palladium on Metal Carbides". Germany. https://doi.org/10.1002/anie.201900781.
@article{osti_1504498,
title = {Enhancing Activity and Reducing Cost for Electrochemical Reduction of CO 2 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 = {Abstract Electrochemical CO 2 reduction reaction (CO 2 RR) 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 2 RR 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 2 RR 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 2 RR environment. DFT calculations reveal that the TMC substrates modify the binding energies of key intermediates on supported PdH. This work suggests the prospect of using TMCs as low‐cost and stable substrates to support and modify Pd for enhanced CO 2 RR activity.},
doi = {10.1002/anie.201900781},
url = {https://www.osti.gov/biblio/1504498}, journal = {Angewandte Chemie (International Edition)},
issn = {1433-7851},
number = 19,
volume = 58,
place = {Germany},
year = {Mon May 06 00:00:00 EDT 2019},
month = {Mon May 06 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1002/anie.201900781

Citation Metrics:
Cited by: 105 works
Citation information provided by
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Works referenced in this record:

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