Acid-Stable Cu Cluster Precatalysts Enable High Energy and Carbon Efficiency in CO<sub>2</sub> Electroreduction
The electrochemical reduction of CO<sub>2</sub> in acidic media offers the advantage of high carbon utilization, but achieving high selectivity to C<sub>2+</sub> products at a low overpotential remains a challenge. We identified the chemical instability of oxide-derived Cu catalysts as a reason that advances in neutral/alkaline electrolysis do not translate to acidic conditions. In acid, Cu ions leach from Cu oxides, leading to the deactivation of the C<sub>2+</sub>-active sites of Cu nanoparticles. This prompted us to design acid-stable Cu cluster precatalysts that are reduced in situ to active Cu nanoparticles in strong acid. Operando Raman and X-ray spectroscopy indicated that the bonding between the Cu cluster precatalyst ligand and in situ formed Cu nanoparticles preserves a high density of undercoordinated Cu sites, resulting in a C<sub>2</sub>H<sub>4</sub> Faradaic efficiency of 62% at a low overpotential. The result is a 1.4-fold increase in energy efficiency compared with previous acidic CO<sub>2</sub>-to-C<sub>2+</sub> electrocatalytic systems.
Authors
- Mingjiang Zhong
- Yang Bai (ORCID: https://orcid.org/0000-0002-1643-3770)
- Jianan Erick Huang (ORCID: https://orcid.org/0000-0001-5872-3680)
- Rui Kai Miao (ORCID: https://orcid.org/0000-0002-0542-0683)
- Weiyan Ni (ORCID: https://orcid.org/0000-0003-0234-4483)
- Panagiotis Papangelakis (ORCID: https://orcid.org/0000-0003-3634-8538)
- Edward Hartley Sargent (ORCID: https://orcid.org/0000-0003-0396-6495)
- Yongxiang Liang (ORCID: https://orcid.org/0009-0003-6921-0102)
- Roham Dorakhan (ORCID: https://orcid.org/0000-0001-8104-7174)
- Tartela Alkayyali (ORCID: https://orcid.org/0000-0003-3895-8700)
- Yanna Chen (ORCID: https://orcid.org/0000-0001-7937-4395)
- Ali Shayesteh Zeraati (ORCID: https://orcid.org/0000-0003-3534-6792)
- Jiheon Kim (ORCID: https://orcid.org/0000-0002-8681-6793)
- David Sinton (ORCID: https://orcid.org/0000-0003-2714-6408)
- Débora Motta Meira (ORCID: https://orcid.org/0000-0002-7529-2736)
- Eui Dae Jung (ORCID: https://orcid.org/0000-0003-4848-0931)
- Sungjin Park (ORCID: https://orcid.org/0000-0002-7631-3500)
- Shijie Liu (ORCID: https://orcid.org/0000-0003-1947-6001)
- Li Feng (ORCID: https://orcid.org/0000-0001-5665-6103)
- Junwoo Lee (ORCID: https://orcid.org/0000-0002-8095-1724)
- Yiqing Chen (ORCID: https://orcid.org/0000-0002-2686-5593)
- Dongha Kim (ORCID: https://orcid.org/0000-0002-8072-9808)
- Peihao Li (ORCID: https://orcid.org/0000-0003-1204-7562)
- Byoung‐Hoon Lee (ORCID: https://orcid.org/0000-0002-0482-2859)
Institutions
- Northwestern University (US)
- Argonne National Laboratory (US)
- University of Toronto (CA)
- Korea University (KR)
- Yale University (US)
- Ajou University (KR)
- Canadian Light Source (Canada) (CA)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-09-27
- DOI
- https://doi.org/10.1021/jacs.4c09230
- Citations
- 30
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 3.07
Funders
- Camille and Henry Dreyfus Foundation
- Ontario Research Foundation
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- National Research Foundation of Korea
- Total
- Natural Sciences and Engineering Research Council of Canada