Bond-Level Dipole Moment Engineering Enables Dual Locking of Lattice Oxygen for Stable CO2-to-Ethylene Electroreduction
Junyue Yin, Hongjing Wang, Jing Wang, Weikun Ren, Jialin Cao, Wenrui Jin, Guixi Wang, Kang Ji, Shiyu Wang, Wanlong Bai, Jingyu Wu, Chao Yi, Baiyu Ren, Zhiyu Yang, Yi-Ming YanAbstract
Copper-based electrocatalysts are highly promising for CO2-to-ethylene conversion, yet their performance degrades because lattice oxygen is lost and Cu+ is reduced to Cu0 under cathodic conditions. To address this challenge, we employed a bond-level dipole moment engineering strategy to stabilize lattice oxygen in Al-doped Cu2O. The oxophilic Al dopant enables a dual-locking mechanism through direct Al–O anchoring and enhanced neighboring Cu–O interactions by increasing the dipole moment. DFT calculations show that Al incorporation lowers antibonding orbital occupancy in Cu+ 3d–O 2p hybridized states, thereby suppressing lattice oxygen leaching. As a result, Al-Cu2O delivers a C2H4 Faradaic efficiency of 37.0%, compared with 20.5% for pristine Cu2O, and maintains stable operation for 50 h. This work supports bond-level dipole moment as a theoretical descriptor for catalyst stability and provides insights into stabilizing oxygen-containing electrocatalysts.