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中文摘要：
氧还原反应（ORR）是一个复杂的过程,尤其在碱性电解液中,炭载型催化剂表面的ORR路径尤为复杂,因为碳本身可以催化ORR以二电子转移过程发生,产生过氧化氢,继而过氧化氢或者发生化学分解生成氧气（HODR）,或者发生电化学还原生成OH（HORR）.本文详细研究了ORR在常用氧化锰催化剂表面的反应路径.通过比较HODR和HORR的转换频率发现,尽管利用旋转环盘电极方法得到的表观电子转移数接近4,真实的ORR主要是2电子过程,反应生成的过氧化氢继而大部分发生化学分解生成氧气.该结果有助于理解碱性电解质中炭载型过渡金属氧化物电催化剂对ORR的催化行为.
英文摘要：
The oxygen reduction reaction（ORR]is a complex process.This is particularly the case for carbon-supported electrocatalysts in alkaline electrolytes,because carbon can catalyze the ORR via a two-electron transfer to generate hydroperoxide（HO2^-],which subsequently undergoes either chemical decomposition to generate O2 and OH-（HODR） or electrochemical reduction to OH-（HORR].In this study,we elucidated the ORR pathway on a series of carbon-supported manganese oxides,which have been extensively studied as electrocatalysts in alkaline electrolytes.A comparison of the turnover frequencies of the HODR and HORR showed that although an apparent four-electron transfer process was identified when the HO2^- yield was measured using the rotating ring disk electrode technique,the real ORR pathway involved a two-electron transfer process to generate HO2^-,with subsequent chemical decomposition of HO2^-.These results will help us to understand the intrinsic catalytic behavior of carbon-supported transition-metal oxides for the ORR in alkaline electrolytes.
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