Cooperative promotion of electroreduction of CO to <i>n</i>-propanol by *CO enrichment and proton regulation
The CO<sub>2</sub>/CO electroreduction reaction (CO<sub>2</sub>RR/CORR) to liquid products presents an enticing pathway to store intermittent renewable electricity. However, the selectivity for desirable high-value C<sub>3</sub> products, such as <i>n</i>-propanol, remains unsatisfactory in the CO<sub>2</sub>RR/CORR. Here, we report that *CO enrichment and proton regulation cooperatively enhance C<sub>1</sub>-C<sub>2</sub> coupling by increasing CO pressure and utilizing proton sponge modification, promoting the production of <i>n</i>-propanol over a Cu<sup>0</sup>/Cu<sup>+</sup> nanosheet catalyst in the CORR. We obtain an impressive faradaic efficiency (FE) of 44.0% ± 2.3% for <i>n</i>-propanol at a low potential of -0.44 V <i>vs.</i> reversible hydrogen electrode (RHE) under 3 bar CO. Experimental results demonstrated that *H intermediates could be regulated by proton sponge modification. <i>In situ</i> characterization combined with density functional theory (DFT) calculations validate that Cu<sup>+</sup> species exist stably in proton sponge-modified Cu-based catalysts along with appropriate *CO coverage. This design facilitates the potential-determining C<sub>1</sub>-C<sub>1</sub> and C<sub>1</sub>-C<sub>2</sub> coupling steps and contributes to the <i>n</i>-propanol production.
Authors
- Cheng Li (ORCID: https://orcid.org/0000-0003-3166-2077)
- Olga A. Syzgantseva (ORCID: https://orcid.org/0000-0002-0270-4621)
- Linxiao Cui
- J. Li (ORCID: https://orcid.org/0009-0009-1397-2734)
- Lingzhi Ding
- Yangyang Dong (ORCID: https://orcid.org/0009-0005-3757-8484)
- Jun Li (ORCID: https://orcid.org/0000-0001-9307-1809)
- Jinyu Ye (ORCID: https://orcid.org/0000-0003-0521-633X)
- Jin‐Chao Dong (ORCID: https://orcid.org/0000-0001-7776-6360)
- Shuliang Yang (ORCID: https://orcid.org/0000-0002-2428-3936)
- Nan Fang (ORCID: https://orcid.org/0009-0005-5005-5573)
- Işıl Akpınar (ORCID: https://orcid.org/0000-0002-3522-4974)
- Bingxing Zhang (ORCID: https://orcid.org/0009-0002-4214-6799)
- Yuan Jiang (ORCID: https://orcid.org/0000-0003-1211-6812)
- Tianwei Xue (ORCID: https://orcid.org/0000-0001-6006-2797)
- Maria A. Syzgantseva (ORCID: https://orcid.org/0000-0001-8070-104X)
- Jianling Zhang (ORCID: https://orcid.org/0000-0002-2648-7529)
- Jie Zhang (ORCID: https://orcid.org/0000-0002-7693-6388)
- Jian‐Feng Li (ORCID: https://orcid.org/0000-0003-1598-6856)
- Peng Li (ORCID: https://orcid.org/0000-0003-0438-7209)
- Buxing Han (ORCID: https://orcid.org/0000-0003-0440-809X)
- Rongxing Qiu (ORCID: https://orcid.org/0009-0001-3205-9600)
Institutions
- Northwestern University (US)
- Peoples' Friendship University of Russia (RU)
- D. Mendeleyev University of Chemical Technology of Russia (RU)
- Zhejiang University of Science and Technology (CN)
- Xiamen University (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
- École Polytechnique Fédérale de Lausanne (CH)
- Zhejiang University (CN)
Publication Details
- Journal
- Chemical Science
- Published
- 2025-01-01
- DOI
- https://doi.org/10.1039/d5sc00274e
- Citations
- 12
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 4.36
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Fujian Province
- Xiamen University
- Fundamental Research Funds for the Central Universities