Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction

De Luna, Phil; Quintero-Bermudez, Rafael; Dinh, Cao-Thang; Ross, Michael B.; Bushuyev, Oleksandr S.; Todorović, Petar; Regier, Tom; Kelley, Shana O.; Yang, Peidong; Sargent, Edward H.

doi:10.1038/s41929-017-0018-9

Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction

Journal Article · Mon Jan 15 00:00:00 EST 2018 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-017-0018-9· OSTI ID:1465700

^[1]; Quintero-Bermudez, Rafael ^[2]; Dinh, Cao-Thang ^[2]; ^[3]; Bushuyev, Oleksandr S. ^[2]; Todorović, Petar ^[2]; Regier, Tom ^[4]; Kelley, Shana O. ^[2]; Yang, Peidong ^[5]; Sargent, Edward H. ^[6]

Univ. of Toronto, ON (Canada); Canadian Institute for Advanced Research, Toronto, ON (Canada). Bio-inspired Solar Energy Program; Univ. of California, Berkeley, CA (United States)
Univ. of Toronto, ON (Canada)
Canadian Institute for Advanced Research, Toronto, ON (Canada). Bio-inspired Solar Energy Program; Univ. of California, Berkeley, CA (United States)
Canadian Light Source Inc. (CLSI), Saskatoon, SK (Canada)
Canadian Institute for Advanced Research, Toronto, ON (Canada). Bio-inspired Solar Energy Program; Univ. of California, Berkeley, CA (United States). Kavli Energy Nanosciences Institute; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Canadian Institute for Advanced Research, Toronto, ON (Canada). Bio-inspired Solar Energy Program; Univ. of Toronto, ON (Canada)

We present that the reduction of carbon dioxide to renewable fuels and feedstocks offers opportunities for large-scale, long-term energy storage. The synthesis of efficient CO₂ reduction electrocatalysts with high C2:C1 selectivity remains a field of intense interest. Here we present electro-redeposition, the dissolution and redeposition of copper from a sol-gel, to enhance copper catalysts in terms of their morphology, oxidation state and consequent performance. We utilized in situ soft X-ray absorption spectroscopy to track the oxidation state of copper under CO₂ reduction conditions with time resolution. The sol-gel material slows the electrochemical reduction of copper, enabling control over nanoscale morphology and the stabilization of Cu⁺ at negative potentials. CO₂ reduction experiments, in situ X-ray spectroscopy and density functional theory simulations revealed the beneficial interplay between sharp morphologies and Cu⁺ oxidation state. Finally, the catalyst exhibits a partial ethylene current density of 160 mA cm^-2(-1.0 V versus reversible hydrogen electrode) and an ethylene/methane ratio of 200.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1465700

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 2 Vol. 1; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction

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