Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes

Chang, Qiaowan; Kim, Jeonghyeon; Lee, Ji Hoon; Kattel, Shyam; Chen, Jingguang G.; Choi, Sang‐Il; Chen, Zheng

doi:10.1002/smll.202005305

Title: Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes

Journal Article · Tue Nov 17 00:00:00 EST 2020 · Small

DOI:https://doi.org/10.1002/smll.202005305· OSTI ID:1749900

^[1]; Kim, Jeonghyeon ^[2];

^[3]; Kattel, Shyam ^[4];

^[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)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; AC02-05CH11231; FG02-13ER16381; NRF-2018R1C1B6004272, 2009-0082580; ACI-1548562; DE‐AC02‐ 05CH11231

OSTI ID:: 1749900

Alternate ID(s):: OSTI ID: 1804832

Report Number(s):: BNL-220739-2020-JAAM

Journal Information:: Small, Vol. 16, Issue 49; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
carbon dioxide reduction reaction
syngas
palladium hydride
nanocubes
Density Functional theory

Title: Boosting Activity and Selectivity of CO2 Electroreduction by Pre-Hydridizing Pd Nanocubes

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