Tuning catalyst-support interactions enable steering of electrochemical CO <sub>2</sub> reduction pathways
Tuning of catalyst-support interactions potentially offers a powerful means to control activity. However, rational design of the catalyst support is challenged by a lack of clear property-activity relationships. Here, we uncover how the electronegativity of a support influences reaction pathways in electrochemical CO<sub>2</sub> reduction. This was achieved by creating a model system consisting of Cu nanoparticles hosted on a series of carbon supports, each with a different heteroatom dopant of varying electronegativity. Notably, we discovered that dopants with high electronegativity reduce the electron density on Cu and induce a selectivity shift toward multicarbon (C<sub>2+</sub>) products. With this design principle, we built a composite Cu and F-doped carbon catalyst that achieves a C<sub>2+</sub> Faradaic efficiency of 82.5% at 400 mA cm<sup>-2</sup>, with stable performance for 44 hours. Using simulated flue gas, the catalyst attains a C<sub>2+</sub> FE of 27.3%, which is a factor of 5.3 times higher than a reference Cu catalyst.
Authors
- Jinfeng Jia
- Wan Ru Leow (ORCID: https://orcid.org/0000-0002-8189-4813)
- Yiwei Shen (ORCID: https://orcid.org/0009-0009-2753-1155)
- Shibo Xi (ORCID: https://orcid.org/0000-0002-8521-3237)
- Ji‐Guang Zhang (ORCID: https://orcid.org/0000-0001-7343-4609)
- Bernt Johannessen (ORCID: https://orcid.org/0000-0002-3027-0816)
- Yanwei Lum (ORCID: https://orcid.org/0000-0001-7261-2098)
- Sung‐Fu Hung (ORCID: https://orcid.org/0000-0002-7423-2723)
- Tanmay Ghosh (ORCID: https://orcid.org/0000-0003-0532-2407)
- Zainul Aabdin (ORCID: https://orcid.org/0000-0002-0436-1327)
- Mingsheng Zhang (ORCID: https://orcid.org/0000-0001-7516-3507)
- Yuke Li (ORCID: https://orcid.org/0000-0003-0162-5072)
- Sibo Wang (ORCID: https://orcid.org/0000-0003-2656-9169)
- Ping Luo
- Ziyu Mi
- Meng Wang (ORCID: https://orcid.org/0009-0009-6648-6203)
Institutions
- Agency for Science, Technology and Research (SG)
- Australian Nuclear Science and Technology Organisation (AU)
- National Yang Ming Chiao Tung University (TW)
- National University of Singapore (SG)
- University of Wollongong (AU)
- Australian Synchrotron (AU)
- Institute of High Performance Computing (SG)
- Institute of Materials Research and Engineering (SG)
Publication Details
- Journal
- Science Advances
- Published
- 2025-04-02
- DOI
- https://doi.org/10.1126/sciadv.ado5000
- Citations
- 14
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 5.09