电合成
化学
电解质
电极
电子转移
标准氢电极
无机化学
电化学
可逆氢电极
质子耦合电子转移
吸附
光化学
物理化学
参比电极
作者
Fan Yu,Yuxin Chen,Wangxin Ge,Dong Liu,Yanbin Qi,Cheng Lian,Xiao‐Dong Zhou,Honglai Liu,Zhen Liu,Hongliang Jiang,Chunzhong Li
摘要
Electrocatalytic reactions taking place at the electrified electrode–electrolyte interface involve processes of proton-coupled electron transfer. Interfacial protons are delivered to the electrode surface via a H2O-dominated hydrogen-bond network. Less efforts are made to regulate the interfacial proton transfer from the perspective of interfacial hydrogen-bond network. Here, we present quaternary ammonium salt cationic surfactants as electrolyte additives for enhancing the H2O2 selectivity of the oxygen reduction reaction (ORR). Through in situ vibrational spectroscopy and molecular dynamics calculation, it is revealed that the surfactants are irreversibly adsorbed on the electrode surface in response to a given bias potential range, leading to the weakening of the interfacial hydrogen-bond network. This decreases interfacial proton transfer kinetics, particularly at high bias potentials, thus suppressing the 4-electron ORR pathway and achieving a highly selective 2-electron pathway toward H2O2. These results highlight the opportunity for steering H2O-involved electrochemical reactions via modulating the interfacial hydrogen-bond network.
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