Results
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