Dissecting Critical Factors for Electrochemical CO2 Reduction on Atomically Precise Au Nanoclusters

Li, Site; Nagarajan, Anantha Venkataraman; Du, Xiangsha; Li, Yingwei; Liu, Zhongyu; Kauffman, Douglas R.; Mpourmpakis, Giannis; Jin, Rongchao

doi:10.1002/anie.202211771

Dissecting Critical Factors for Electrochemical CO₂ Reduction on Atomically Precise Au Nanoclusters

Journal Article · Tue Oct 25 00:00:00 EDT 2022 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202211771· OSTI ID:1899592

Li, Site ^[1]; Nagarajan, Anantha Venkataraman ^[2]; Du, Xiangsha ^[3]; Li, Yingwei ^[3]; Liu, Zhongyu ^[3]; Kauffman, Douglas R. ^[4]; Mpourmpakis, Giannis ^[2]; ^[3]

Carnegie Mellon Univ., Pittsburgh, PA (United States); National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
Univ. of Pittsburgh, PA (United States)
Carnegie Mellon Univ., Pittsburgh, PA (United States)
National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)

Here, this work investigates the critical factors impacting electrochemical CO₂ reduction reaction (CO₂RR) using atomically precise Au nanoclusters (NCs) as electrocatalysts. First, the influence of size on CO₂RR is studied by precisely controlling NC size in the 1–2.5 nm regime. We find that the electrocatalytic CO partial current density increases for smaller NCs, but the CO Faradaic efficiency (FE) is not directly associated with the NC size. This indicates that the surface-to-volume ratio, i.e. the population of active sites, is the dominant factor for determining the catalytic activity, but the selectivity is not directly impacted by size. Second, we compare the CO₂RR performance of Au₃₈ isomers (Au₃₈Q and Au₃₈T) to reveal that structural rearrangement of identical size NCs can lead to significant changes in both CO₂RR activity and selectivity. Au₃₈Q shows higher activity and selectivity towards CO than Au₃₈T, and density functional theory (DFT) calculations reveal that the average formation energy of the key *COOH intermediate on the proposed active sites is significantly lower on Au₃₈Q than Au₃₈T. These results demonstrate how the structural isomerism can impact stabilization of reaction intermediates as well as the overall CO₂RR performance of identical size Au NCs. Overall, this work provides important structure–property relationships for tailoring the NCs for CO₂RR.

View Accepted Manuscript (DOE)

Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1899592

Report Number(s):: DOE/NETL-2022/3328

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 47 Vol. 61; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 reduction
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Dissecting Critical Factors for Electrochemical CO2 Reduction on Atomically Precise Au Nanoclusters

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Dissecting Critical Factors for Electrochemical CO₂ Reduction on Atomically Precise Au Nanoclusters