Shifting electrochemical oxygen reduction towards 2e– pathway to hydrogen peroxide (H2O2), instead of the traditional 4e– to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm−2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e–/4e– ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e–, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.
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机译:作为一种生成H2O2的绿色方法,将电化学氧还原方法从2e – sup>途径转移到过氧化氢(H2O2)而不是传统的4e – sup>途径转移到水中变得越来越重要。在这里,通过灵活控制碳纳米管中不同过渡金属单原子配位上的氧还原途径,我们发现Fe-CO是一种有效的H2O2催化剂,相对于0.1 M KOH中可逆的氢电极,其前所未有的起效为0.822 V,可提供0.1 mA cm −2 sup> H2O2电流,在碱性和中性pH值下H2O2的选择性都高于95%。通过不同的金属中心或邻近的准金属配位,实现了2e – sup> / 4e – sup> ORR途径的大范围调节。密度泛函理论计算表明,与众所周知的4e – sup>的Fe-C-N形成鲜明对比的是Fe-C-O基元是H2O2途径的原因。该铁单原子催化剂证明了有效的水消毒作为代表性的应用。
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