Steering Ethylene Electrosynthesis by Controlling Interfacial Water Orientation
Abstract
ABSTRACT Controlling reaction pathway via solvent polarization dynamics remains a grand challenge in catalysis due to elusive interfacial kinetic regulation mechanisms. Here, we resolve this dilemma by establishing interfacial water orientation that directly couples H 2 O polarization with reaction pathway bifurcation. Using electrocatalytic CO 2 reduction as a typical platform, we demonstrate that precisely engineered H‐down water alignment, achieved via adaptive subsurface tuning (AST) strategy of Ga‐doped Cu catalysts, dynamically regulates proton transfer directionality and intermediate stabilization. The optimized Ga/Cu catalyst achieved a Faradaic efficiency (FE) of 68.8% for ethylene at 800 mA cm −2 , surpassing ethanol production by 8.2‐fold, and the current density was among the highest reported for catalysts with high ethylene FE. Detailed experimental studies and theoretical calculations corroborate that H‐down alignment enhanced *H availability, directing protons to selectively cleave the C─O bond of *CHCOH intermediates over hydrogenation pathways, yielding high ethylene FE and current density. These findings establish interfacial water orientation as a pivotal descriptor for steering C─C coupling selectivity in electrocatalysis, offering a rational design principle for efficient electroreduction systems.
Article Details
Authors (17)
Xinning Song
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Libing Zhang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Xiaodong Ma
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Limin Wu
School of Chemistry and Chemical Engineering
Xingxing Tan
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Weixiang Li
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Chaofeng Zheng
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Shunhan Jia
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Ruhan Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Xing Tong
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Qingli Qian
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Jiao Mu
Beijing National Laboratory for Molecular Sciences, Huairou Research Center
Rongjuan Feng
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Lin Hu
The High Magnetic Field Laboratory, Hefei Institutes of Physical Science
Xiaolong Wang
Xiaofu Sun
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,