Electrochimica Acta ( IF 5.5 ) Pub Date : 2022-08-26 , DOI: 10.1016/j.electacta.2022.141091
Ming Cheng , Zongge Li , Tongxin Xu , Yuxin Mao , Ying Zhang , Guoxin Zhang , Zifeng Yan
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Synthesis of H2O2 via 2e− O2 reduction or 2e− H2O oxidation has been widely acknowledged as promising alteratives to the energy-intensive anthraquinone processes. Herein, we report that the 2e− O2 reduction and 2e− H2O oxidation reactions, for the first time, can be efficiently promoted on CeO2 (100) facets, while majority of previous CeO2 materials are utilized overwhelmingly as catalyst substrates. Electrochemical measurements indicate that CeO2 nanocubes (NCs) deliver very high H2O2 selectivity of 83% and faradic efficiency of 95.3% for 2e− O2 reduction. Its H2O2 yield rate at 0.5 V (vs. RHE) reaches 632 mmol gcat−1 h−1, which exceeds the performance of facet-unspecified CeO2 nanodots (NDs) in this work and many noble metal- or carbon-based electrocatalysts in previous literatures. Furthermore, it also shows a high efficiency of 66% for 2e− H2O oxidation. When assembled into flow cell reactor, the CeO2 NCs can obtain a total H2O2 yield of 4.6 mol gcat.−1 h−1, and manage stable faradic efficiency (> 85%) in wide voltage range. Our work may inspire further investigation of rare earth metal oxide-based materials for 2e− oxygen electrocatalysis.
中文翻译:

在 CeO2 纳米立方体上进行高效的整体 2e-氧电解生成 H2O2
通过 2e - O 2还原或 2e - H 2 O 氧化合成 H 2 O 2已被广泛认为是能源密集型蒽醌过程的有希望的替代品。在此,我们首次报道了 2e - O 2还原和 2e - H 2 O 氧化反应可以在 CeO 2 (100) 晶面上有效地促进,而之前的大多数 CeO 2材料被压倒性地用作催化剂基材. 电化学测量表明,CeO 2纳米立方体 (NC) 可提供非常高的 H 22e - O 2还原的O 2选择性为 83%,法拉第效率为 95.3% 。其在 0.5 V 时的 H 2 O 2产率(与 RHE 相比)达到 632 mmol g cat -1 h -1,超过了这项工作中未指定刻面的 CeO 2纳米点 (NDs) 和许多贵金属或碳的性能以前文献中的基电催化剂。此外,它还显示出 66% 的 2e - H 2 O 氧化效率。当组装到流通池反应器中时,CeO 2 NCs 可以获得4.6 mol g cat的总 H 2 O 2产率。-1 h -1,并在宽电压范围内管理稳定的法拉第效率 (> 85%)。我们的工作可能会激发对用于 2e -氧电催化的稀土金属氧化物基材料的进一步研究。