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High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
Nature Catalysis ( IF 37.8 ) Pub Date : 2018-01-15 , DOI: 10.1038/s41929-017-0017-x
Zhiyi Lu , Guangxu Chen , Samira Siahrostami , Zhihua Chen , Kai Liu , Jin Xie , Lei Liao , Tong Wu , Dingchang Lin , Yayuan Liu , Thomas F. Jaramillo , Jens K. Nørskov , Yi Cui

Hydrogen peroxide (H2O2) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H2O2 involves an energy-intensive anthraquinone process. The electrochemical synthesis of H2O2 from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H2O2 production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. The density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments.



中文翻译:

氧化碳材料催化的氧气高效还原为过氧化氢

过氧化氢(H 2 O 2)是有价值的化学物质,具有广泛的应用范围,但是H 2 O 2的当前工业合成涉及高能耗的蒽醌工艺。由氧还原电化学合成H 2 O 2为现场应用提供了另一种途径。该方法的效率在很大程度上取决于鉴定具有高活性和选择性的具有成本效益的催化剂。在这里,我们展示了一种通过丰富的碳材料的表面氧化来显着提高H 2 O 2的活性和选择性(〜90%)的简便而通用的催化剂开发方法。通过电化学氧还原生产。我们发现活性和选择性都与催化剂的氧含量正相关。密度泛函理论计算表明,与几个氧官能团(–COOH和C–OC–C)相邻的碳原子是通过双电子途径进行氧还原反应的活性位点,并进一步受到一系列控制的支持实验。

更新日期:2018-01-16
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