Tuning catalyst-support interactions enable steering of electrochemical CO 2 reduction pathways

作者：Meng Wang, Yuke Li, Jinfeng Jia, Tanmay Ghosh, Ping Luo, Yu-Jhih Shen, Sibo Wang, Ji‐Guang Zhang, Ji‐Guang Zhang, Shibo Xi, Ziyu Mi, Mingsheng Zhang, Wan Ru Leow, Bernt Johannessen, Zainul Aabdin, Sung‐Fu Hung, Jia Zhang, Jia Zhang, Yanwei Lum · 发表于：Science Advances · 年份：2025 · DOI：10.1126/sciadv.ado5000 · 被引用次数：22 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Covalent Organic Framework Applications

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 2 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 2+ ) products. With this design principle, we built a composite Cu and F-doped carbon catalyst that achieves a C 2+ Faradaic efficiency of 82.5% at 400 mA cm −2 , with stable performance for 44 hours. Using simulated flue gas, the catalyst attains a C 2+ FE of 27.3%, which is a factor of 5.3 times higher than a reference Cu catalyst.