Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene
The electrocatalytic conversion of carbon dioxide (CO<sub>2</sub>) to ethylene (C<sub>2</sub>H<sub>4</sub>) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified a praseodymium (Pr) single-atom alloy embedded in a copper (Cu) catalyst (Pr@Cu) that exhibits superior CO<sub>2</sub> activation and a remarkably low energy barrier for asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves a C<sub>2</sub>H<sub>4</sub> Faradaic efficiency (FE) of 64.2% at -1.6 V versus the reversible hydrogen electrode (RHE) under a high current density of 1200 mA cm<sup>-2</sup> in the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). Furthermore, when integrated into a 100 cm<sup>2</sup> membrane electrode assembly (MEA) electrolyzer, Pr@Cu-2 demonstrates robust performance, maintaining a continuous C<sub>2</sub>H<sub>4</sub> production rate of 21.3 mL min<sup>-1</sup> at 20 A for over 200 h. This work provides fundamental insights into the role of Pr single-atom alloys in the CO<sub>2</sub>RR and highlights their potential for scalable C<sub>2</sub>H<sub>4</sub> electrosynthesis.
Authors
- Fei Song (ORCID: https://orcid.org/0000-0002-6408-7796)
- Ruijuan Qi (ORCID: https://orcid.org/0000-0003-2305-0505)
- Bao Yu Xia (ORCID: https://orcid.org/0000-0002-2054-908X)
- Wei Guo (ORCID: https://orcid.org/0000-0002-1378-0048)
- Yuye Zhao (ORCID: https://orcid.org/0009-0001-3618-4716)
- N. Liu
- Hongming Wang (ORCID: https://orcid.org/0000-0002-2207-8015)
- Jiwen Chen (ORCID: https://orcid.org/0000-0002-9969-7578)
- Fuqing Yu (ORCID: https://orcid.org/0000-0002-0003-4126)
- Yanteng Xiao (ORCID: https://orcid.org/0000-0001-6730-5907)
- Yuanjie Pang (ORCID: https://orcid.org/0000-0003-1328-3700)
- Bo You (ORCID: https://orcid.org/0000-0003-1849-0418)
- Ziyun Wang (ORCID: https://orcid.org/0000-0002-2817-8367)
- Tao Yao (ORCID: https://orcid.org/0000-0001-8699-8294)
- Deyu Zhu
- Chenfeng Xia
Institutions
- University of Science and Technology of China (CN)
- Nanchang University (CN)
- University of Auckland (NZ)
- Chinese Academy of Sciences (CN)
- Shanghai Advanced Research Institute (CN)
- Advanced Research Institute (US)
- Wuhan National Laboratory for Optoelectronics (CN)
- Advanced Materials and Devices (United States) (US)
- National Synchrotron Radiation Laboratory (CN)
- Huazhong University of Science and Technology (CN)
- East China Normal University (CN)
- Sungkyunkwan University (KR)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-04-25
- DOI
- https://doi.org/10.1021/jacs.5c02896
- Citations
- 54
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 19.63
Funders
- National Natural Science Foundation of China
- National Key Research and Development Program of China