High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
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DOI：
10.1038/s41929-017-0017-x
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发表时间：
2018-02-01
期刊：
影响因子：
37.8
通讯作者：
Cui, Yi
中科院分区：
文献类型：
--
作者：
Lu, Zhiyi;Chen, Guangxu;Cui, Yi
过氧化氢（H2 O2）是一种有价值的化学品，具有广泛的应用，但目前的工业合成H2 O2涉及能源密集型蒽醌工艺。氧气还原电化学合成H2 O2为现场应用提供了一种替代途径;该过程的效率在很大程度上取决于确定具有高活性和选择性的具有成本效益的催化剂。在这里，我们展示了一个简单的和一般的方法，通过丰富的碳材料的表面氧化催化剂的发展，显着提高活性和选择性（类似于90%）的H2 O2生产的电化学氧还原。发现催化剂的活性和选择性与氧含量呈正相关。密度泛函理论计算表明，与多个含氧官能团（-COOH和C-O-C）相邻的碳原子是氧还原反应的活性中心，并通过一系列控制实验进一步证实了这一点.
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 (similar to 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.