Amorphous CeO2–Cu Heterostructure Enhances CO2 Electroreduction to Multicarbon Alcohols

Kou, Tianyi; Wang, Shanwen; Yang, Shaokang; Ren, Qiu; Ball, Riley; Rao, Dewei; Chiovoloni, Samuel; Lu, Jennifer Q.; Zhang, Zhonghua; Duoss, Eric B.; Li, Yat

doi:10.1021/acsmaterialslett.2c00506

Amorphous CeO₂–Cu Heterostructure Enhances CO₂ Electroreduction to Multicarbon Alcohols

Journal Article · Mon Sep 12 00:00:00 EDT 2022 · ACS Materials Letters

DOI:https://doi.org/10.1021/acsmaterialslett.2c00506· OSTI ID:1903453

^[1]; Wang, Shanwen ^[2]; Yang, Shaokang ^[3]; Ren, Qiu ^[2]; Ball, Riley ^[2]; ^[3]; Chiovoloni, Samuel ^[4]; ^[4]; ^[5]; Duoss, Eric B. ^[6]; ^[2]

Univ. of California, Santa Cruz, CA (United States); Shandong Univ., Weihai (China)
Univ. of California, Santa Cruz, CA (United States)
Jiangnan Univ., Zhenjiang (China)
Univ. of California, Merced, CA (United States)
Shandong Univ., Jinan (China)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Electrochemical conversion of carbon dioxide (CO₂) gas to value-added chemicals such as multicarbon (C₂₊) alcohols is a promising and attractive decarbonization strategy. However, there are tremendous challenges in tuning the intrinsic activity and selectivity of the catalysts to produce C₂₊ alcohols. In this work, we prepared a CeO₂–Cu composite catalyst via a combination of metallurgy and dealloying method. The interfacial sites of amorphous CeO₂–Cu heterostructure improve the adsorption of key reaction intermediates *CO and promote the C–C coupling. Significantly, they also stabilize *CH₂CHO at the bifurcation step, steering the reaction pathway toward the formation of C₂₊ alcohols over ethylene. The CeO₂–Cu catalyst achieves a remarkable faradaic efficiency of 32.9% ± 2.6% for C₂₊ alcohols at -0.6 V vs RHE. Overall, this work demonstrates an effective strategy of improving the intrinsic activity and selectivity of the Cu-based catalysts for the generation of C₂₊ alcohols.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: Merced nAnomaterials Center for Energy and Sensing (MACES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1903453

Report Number(s):: LLNL-JRNL-835770; 1054952

Journal Information:: ACS Materials Letters, Journal Name: ACS Materials Letters Journal Issue: 10 Vol. 4; ISSN 2639-4979

Publisher:: ACS PublicationsCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
adsorption
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hydrocarbons

Amorphous CeO2–Cu Heterostructure Enhances CO2 Electroreduction to Multicarbon Alcohols

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Amorphous CeO₂–Cu Heterostructure Enhances CO₂ Electroreduction to Multicarbon Alcohols