High-Pressure Electro-Fenton Driving CH 4 Conversion by O 2 at Room Temperature

• Published in: Journal of the American Chemical Society Vol. 146; no. 9; pp. 5834 - 5842
• Main Authors: Song, Yao, Yang, Xiao, Liu, Huan, Liang, Suxia, Cai, Yafeng, Yang, Wenqiang, Zhu, Kaixin, Yu, Liang, Cui, Xiaoju, Deng, Dehui
• Format: Journal Article
• Language: English
• Published: United States 06-03-2024
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.3c10825

Electrochemical conversion of CH
to easily transportable and value-added liquid fuels is highly attractive for energy-efficient CH
utilization, but it is challenging due to the low reactivity and solubility of CH
in the electrolyte. Herein, we report a high-pressure electro-Fenton (HPEF) strategy to establish a hetero-homogeneous process for the electrocatalytic conversion of CH
by O
at room temperature. In combination with elevation of reactant pressure to accelerate reaction kinetics, it delivers an unprecedented HCOOH productivity of 11.5 mmol h
g
with 220 times enhancement compared to that under ambient pressure. Remarkably, an HCOOH Faradic efficiency of 81.4% can be achieved with an ultralow cathodic overpotential of 0.38 V. The elevated pressure not only promotes the electrocatalytic reduction of O
to H
O
but also increases the reaction collision probability between CH
and •OH, which is in situ generated from the Fe
-facilitated decomposition of H
O
.