Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes
Abstract
Abstract The electrochemical CO 2 reduction reaction (CO 2 RR) to syngas represents a promising solution to mitigate CO 2 emissions and manufacture value‐added chemicals. Palladium (Pd) has been identified as a potential candidate for syngas production via CO 2 RR due to its transformation to Pd hydride under CO 2 RR conditions, however, the pre‐hydridized effect on the catalytic properties of Pd‐based electrocatalysts has not been investigated. Herein, pre‐hydridized Pd nanocubes (PdH 0.40 ) supported on carbon black (PdH 0.40 NCs/C) are directly prepared from a chemical reduction method. Compared with Pd nanocubes (Pd NCs/C), PdH 0.40 NCs/C presented an enhanced CO 2 RR performance due to its less cathodic phase transformation revealed by the in situ X‐ray absorption spectroscopy. Density functional theory calculations revealed different binding energies of key reaction intermediates on PdH 0.40 NCs/C and Pd NCs/C. Study of the size effect further suggests that NCs of smaller sizes show higher activity due to their more abundant active sites (edge and corner sites) for CO 2 RR. The pre‐hydridization and reduced NC size together lead to significantly improved activity and selectivity of CO 2 RR.
- Authors:
-
[1];
[3];
[5];
[2];
[1]
- Univ. of California, San Diego, CA (United States)
- Kyungpook National Univ., Daegu (Korea, Republic of)
- Kyungpook National Univ., Daegu (Korea, Republic of); Columbia Univ., New York, NY (United States)
- Florida A & M University, Tallahassee, FL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); National Science Foundation (NSF)
- OSTI Identifier:
- 1749900
- Alternate Identifier(s):
- OSTI ID: 1804832
- Report Number(s):
- BNL-220739-2020-JAAM
Journal ID: ISSN 1613-6810
- Grant/Contract Number:
- SC0012704; AC02-05CH11231; FG02-13ER16381; NRF-2018R1C1B6004272, 2009-0082580; ACI-1548562; DE‐AC02‐ 05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Small
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 49; Journal ID: ISSN 1613-6810
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; carbon dioxide reduction reaction; syngas; palladium hydride; nanocubes; Density Functional theory
Citation Formats
Chang, Qiaowan, Kim, Jeonghyeon, Lee, Ji Hoon, Kattel, Shyam, Chen, Jingguang G., Choi, Sang‐Il, and Chen, Zheng. Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes. United States: N. p., 2020.
Web. doi:10.1002/smll.202005305.
Chang, Qiaowan, Kim, Jeonghyeon, Lee, Ji Hoon, Kattel, Shyam, Chen, Jingguang G., Choi, Sang‐Il, & Chen, Zheng. Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes. United States. https://doi.org/10.1002/smll.202005305
Chang, Qiaowan, Kim, Jeonghyeon, Lee, Ji Hoon, Kattel, Shyam, Chen, Jingguang G., Choi, Sang‐Il, and Chen, Zheng. Tue .
"Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes". United States. https://doi.org/10.1002/smll.202005305. https://www.osti.gov/servlets/purl/1749900.
@article{osti_1749900,
title = {Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes},
author = {Chang, Qiaowan and Kim, Jeonghyeon and Lee, Ji Hoon and Kattel, Shyam and Chen, Jingguang G. and Choi, Sang‐Il and Chen, Zheng},
abstractNote = {Abstract The electrochemical CO 2 reduction reaction (CO 2 RR) to syngas represents a promising solution to mitigate CO 2 emissions and manufacture value‐added chemicals. Palladium (Pd) has been identified as a potential candidate for syngas production via CO 2 RR due to its transformation to Pd hydride under CO 2 RR conditions, however, the pre‐hydridized effect on the catalytic properties of Pd‐based electrocatalysts has not been investigated. Herein, pre‐hydridized Pd nanocubes (PdH 0.40 ) supported on carbon black (PdH 0.40 NCs/C) are directly prepared from a chemical reduction method. Compared with Pd nanocubes (Pd NCs/C), PdH 0.40 NCs/C presented an enhanced CO 2 RR performance due to its less cathodic phase transformation revealed by the in situ X‐ray absorption spectroscopy. Density functional theory calculations revealed different binding energies of key reaction intermediates on PdH 0.40 NCs/C and Pd NCs/C. Study of the size effect further suggests that NCs of smaller sizes show higher activity due to their more abundant active sites (edge and corner sites) for CO 2 RR. The pre‐hydridization and reduced NC size together lead to significantly improved activity and selectivity of CO 2 RR.},
doi = {10.1002/smll.202005305},
journal = {Small},
number = 49,
volume = 16,
place = {United States},
year = {Tue Nov 17 00:00:00 EST 2020},
month = {Tue Nov 17 00:00:00 EST 2020}
}
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