电合成
过氧化氢
碱金属
化学
无机化学
电流(流体)
金属
电化学
有机化学
电极
物理化学
电气工程
工程类
作者
Peike Cao,Xueyang Zhao,Yanming Liu,Haiguang Zhang,Kun Zhao,Shuo Chen,Hongtao Yu,Dongrui Fan,Nathaniel N. Nichols,Jingguang G. Chen,Quan Xie
标识
DOI:10.1002/ange.202406452
摘要
Acidic H2O2 synthesis through electrocatalytic 2e– oxygen reduction presents a sustainable alternative to the energy‐intensive anthraquinone oxidation technology. Nevertheless, acidic H2O2 electrosynthesis suffers from low H2O2 Faradaic efficiencies primarily due to the competing reactions of 4e– oxygen reduction to H2O and hydrogen evolution in environments with high H+ concentrations. Here, we demonstrate the significant effect of alkali metal cations, acting as competing ions with H+, in promoting acidic H2O2 electrosynthesis at industrial‐level currents, resulting in an effective current densities of 50‒421 mA cm‒2 with 84‒100% Faradaic efficiency and a production rate of 856‒7842 μmol cm‐2 h‐1 that far exceeds the performance observed in pure acidic electrolytes or low‐current electrolysis. Finite‐element simulations indicate that high interfacial pH near the electrode surface formed at high currents is crucial for activating the promotional effect of K+. In situ attenuated total reflection Fourier transform infrared spectroscopy and ab initio molecular dynamics simulations reveal the central role of alkali metal cations in stabilizing the key *OOH intermediate to suppress 4e– oxygen reduction through interacting with coordinated H2O.
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