Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Chang, Qiaowan; Lee, Ji Hoon; Liu, Yumeng; Xie, Zhenhua; Hwang, Sooyeon; Marinkovic, Nebojsa S.; Park, Ah-Hyung Alissa; Kattel, Shyam; Chen, Jingguang G.

doi:10.1021/jacsau.1c00487

Title: Electrochemical CO₂ Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

Journal Article · Thu Dec 09 00:00:00 EST 2021 · JACS Au

DOI:https://doi.org/10.1021/jacsau.1c00487· OSTI ID:1837207

Chang, Qiaowan ^[1];

^[2]; Liu, Yumeng ^[1]; Xie, Zhenhua ^[3];

^[3]; Marinkovic, Nebojsa S. ^[1];

^[1]; Kattel, Shyam ^[4];

^[5]

Columbia Univ., New York, NY (United States)
Columbia Univ., New York, NY (United States); Kyungpook National Univ., Daegu (Korea, Republic of)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Florida A & M University, Tallahassee, FL (United States)
Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Electrochemical carbon dioxide reduction reaction (CO₂RR) using copper (Cu)-based catalysts has received significant attention mainly because Cu is an element capable of producing hydrocarbons and oxygenates. One possible way to control the CO₂RR performance at the electrode interface is by modifying catalysts with specific functional groups of different polymeric binders, which are necessary components in the process of electrode fabrication. However, the modification effect of the key functional groups on the CO₂RR activity and selectivity is poorly understood over Cu-based catalysts. In this work, the role of functional groups (e.g., -COOH and -CF₂ groups) in hydrophilic and hydrophobic polymeric binders on the CO₂RR of Cu-based catalysts is investigated using a combination of electrochemical measurements, in-situ characterization and density functional theory (DFT) calculations. DFT results reveal that functional groups influence the binding energies of key intermediates involved in both CO₂RR and the competing hydrogen evolution reaction, consistent with experimental observation of binder-dependent product distributions among formic acid, CO, CH₄, and H₂. This study provides a fundamental understanding that the selection of desired polymeric binders is a useful strategy for tuning the CO₂RR activity and selectivity.

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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 Science Foundation (NSF); National Research Foundation of Korea (NRF); China Scholarship Council

Grant/Contract Number:: SC0012704; 1927336; ACI-1548562; NRF-2021R1G1A1092280; 201806010243

OSTI ID:: 1837207

Report Number(s):: BNL-222517-2021-JAAM

Journal Information:: JACS Au, Vol. 2, Issue 1; ISSN 2691-3704

Publisher:: ACS PublicationsCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Electrochemical CO2 Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder

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Title: Electrochemical CO₂ Reduction Reaction over Cu Nanoparticles with Tunable Activity and Selectivity Mediated by Functional Groups in Polymeric Binder