Tuning catalyst-support interactions enable steering of electrochemical CO <sub>2</sub> reduction pathways
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
Abstract
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.