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- Title
Electrocatalytic Methane Oxidation Greatly Promoted by Chlorine Intermediates.
- Authors
Wang, Qihao; Li, Tengfei; Yang, Chao; Chen, Menghuan; Guan, Anxiang; Yang, Li; Li, Si; Lv, Ximeng; Wang, Yuhang; Zheng, Gengfeng
- Abstract
Renewable energy‐powered methane (CH4) conversion at ambient conditions is an attractive but highly challenging field. Due to the highly inert character of CH4, the selective cleavage of its first C−H bond without over‐oxidation is essential for transforming CH4 into value‐added products. In this work, we developed an efficient and selective CH4 conversion approach at room temperature using intermediate chlorine species (*Cl), which were electrochemically generated and stabilized on mixed cobalt–nickel spinels with different Co/Ni ratios. The lower overpotentials for *Cl formation enabled an effective activation and conversion of CH4 to CH3Cl without over‐oxidation to CO2, and Ni3 at the octahedral sites in the mixed cobalt–nickel spinels allowed to stabilize surface‐bound *Cl species. The CoNi2Ox electrocatalyst exhibited an outstanding yield of CH3Cl (364 mmol g−1 h−1) and a high CH3Cl/CO2 selectivity of over 400 at room temperature, with demonstrated capability of direct CH4 conversion under seawater working conditions.
- Subjects
CHLORINE; METHANE; STEAM reforming; OXIDATION; SPINEL group; CARBON dioxide; SEAWATER
- Publication
Angewandte Chemie, 2021, Vol 133, Issue 32, p17538
- ISSN
0044-8249
- Publication type
Academic Journal
- DOI
10.1002/ange.202105523