Methanol oxidation plays a central role to implement sustainable energy economy, which is restricted by the sluggish reaction kinetics due to the multi‐electron transfer process accompanied by numerous sequential intermediate. In this study, an efficient cascade methanol oxidation reaction is catalyzed by single‐Ir‐atom catalyst at ultra‐low potential (< 0.1 V) with the promotion of the thermal and electrochemical integration in a high temperature polymer electrolyte membrane electrolyzer. At the elevated temperature, the electron deficient Ir site with higher methanol affinity could spontaneous catalyze the CH3OH dehydrogenation to CO under the voltage, then the generated CO and H2 was electrochemically oxidized to CO2 and proton. However, the methanol cannot thermally decompose with the voltage absence, which confirm the indispensable of the coupling of thermal and electrochemical integration for the methanol oxidation. By assembling the methanol oxidation reaction with hydrogen evolution reaction in the HT‐PEME with single‐Ir‐atom catalysts in the anode chamber, a max hydrogen production rate reaches 18 mol gIr‐1 h‐1, which is much greater than that of Ir nanoparticles and commercial Pt/C catalyst. This study also demonstrated the electrochemical MOR activity of the single atom catalysts, which broadens the renewable energy devices and the catalyst design by an integration concept.

中文翻译：

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单 Ir 原子催化剂上的超低电势甲醇氧化

甲醇氧化在实现可持续能源经济中发挥着核心作用，但由于多电子转移过程伴随着大量连续中间体，反应动力学缓慢，制约了甲醇氧化的发展。在这项研究中，单Ir原子催化剂在超低电势（< 0.1 V）下催化了高效的级联甲醇氧化反应，并促进了高温聚合物电解质膜电解槽中的热和电化学集成。在高温下，具有较高甲醇亲和力的缺电子Ir位点在电压作用下自发催化CH3OH脱氢生成CO，然后生成的CO和H2被电化学氧化为CO2和质子。然而，在没有电压的情况下，甲醇不能热分解，这证实了热与电化学集成的耦合对于甲醇氧化是必不可少的。通过在阳极室中使用单 Ir 原子催化剂将甲醇氧化反应与析氢反应组装在 HT-PEME 中，最大产氢速率达到 18 mol gIr-1 h-1，远高于 Ir 的产氢速率。纳米颗粒和商用 Pt/C 催化剂。这项研究还证明了单原子催化剂的电化学MOR活性，通过集成概念拓宽了可再生能源设备和催化剂设计。