Taming the Hydrogen‐Mediated Kinetic Switch for Sulfur‐Tolerant CO <sub>2</sub> Electroreduction
Abstract
ABSTRACT Direct electrochemical conversion of industrial flue gas offers a promising route to carbon neutrality, but it remains limited by trace sulfur dioxide (SO 2 , 10–400 ppm) impurities. These impurities cause rapid catalyst deactivation, particularly under the high reaction rates required for industrial application. Here, we introduce a hydrophobic molecular gate strategy to decouple impurity transport from catalyst deactivation. By regulating the interfacial water solvation structure and proton transfer pathways, this design creates a water‐deficient regime to lock the kinetic switch. As a result, SO 2 is isolated from the hydrogen‐mediated reduction, while the transient water required for efficient CO 2 conversion is preserved. When paired with a lattice‐strained copper catalyst, this architecture allows a scaled‐up 100 cm 2 membrane electrode assembly (MEA) to operate at a total current of 20 A for over 120 h, maintaining an ethylene (C 2 H 4 ) Faradaic efficiency (FE) >56% in simulated flue gas.
Article Details
Authors (10)
Mingzhi Wang
State Key Laboratory of New Textile Materials and Advanced Processing Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology (HUST) Wuhan China
Wensheng Fang
State Key Laboratory of New Textile Materials and Advanced Processing Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology (HUST) Wuhan China
Lebin Cai
State Key Laboratory of New Textile Materials and Advanced Processing Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure School of Chemistry and Chemical Engineering Huazhong University of Science and Technology (HUST) Wuhan China
Deyu Zhu
School of Basic Medical Sciences
Yi Shi
School of Materials Science and Engineering, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, Guangdong Functional Biomaterials Engineering Technology Research Center
Wei Guo
Xiaolong Zhang
State Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science
Bo You
School of Chemistry and Chemical Engineering, State Key Laboratory of Materials Processing and Die & Mould Technology, Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology (HUST), 1037 Luoyu Road, Wuhan 430074, China
Fei Song
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute
Bao Yu Xia
State Key Laboratory of New Textile Materials and Advanced Processing, Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering