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 HO but also increases the reaction collision probability between CH and •OH, which is in situ generated from the Fe-facilitated decomposition of HO.
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http://dx.doi.org/10.1021/jacs.3c10825 | DOI Listing |
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