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通过选择性氧还原电合成过氧化氢:从活性位点工程到器件设计的碳创新

Electrosynthesis of Hydrogen Peroxide through Selective Oxygen Reduction: A Carbon Innovation from Active Site Engineering to Device Design.

作者信息

Zhang Qingran, Chen Yinguang, Pan Jian, Daiyan Rahman, Lovell Emma C, Yun Jimmy, Amal Rose, Lu Xunyu

机构信息

Particles and Catalysis Research Group, School of Chemical Engineering, The University of New South Wales, Sydney, NSW, 2052, Australia.

State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai, 200092, China.

出版信息

Small. 2023 Oct;19(40):e2302338. doi: 10.1002/smll.202302338. Epub 2023 Jun 2.

Abstract

Electrochemical synthesis of hydrogen peroxide (H O ) through the selective oxygen reduction reaction (ORR) offers a promising alternative to the energy-intensive anthraquinone method, while its success relies largely on the development of efficient electrocatalyst. Currently, carbon-based materials (CMs) are the most widely studied electrocatalysts for electrosynthesis of H O via ORR due to their low cost, earth abundance, and tunable catalytic properties. To achieve a high 2e ORR selectivity, great progress is made in promoting the performance of carbon-based electrocatalysts and unveiling their underlying catalytic mechanisms. Here, a comprehensive review in the field is presented by summarizing the recent advances in CMs for H O production, focusing on the design, fabrication, and mechanism investigations over the catalytic active moieties, where an enhancement effect of defect engineering or heteroatom doping on H O selectivity is discussed thoroughly. Particularly, the influence of functional groups on CMs for a 2e -pathway is highlighted. Further, for commercial perspectives, the significance of reactor design for decentralized H O production is emphasized, bridging the gap between intrinsic catalytic properties and apparent productivity in electrochemical devices. Finally, major challenges and opportunities for the practical electrosynthesis of H O and future research directions are proposed.

摘要

通过选择性氧还原反应(ORR)电化学合成过氧化氢(H₂O₂)为能源密集型蒽醌法提供了一种有前景的替代方法,而其成功很大程度上依赖于高效电催化剂的开发。目前,碳基材料(CMs)因其低成本、地球储量丰富和可调节的催化性能,是通过ORR电合成H₂O₂研究最广泛的电催化剂。为了实现高2e ORR选择性,在提高碳基电催化剂性能和揭示其潜在催化机制方面取得了巨大进展。在此,通过总结CMs用于H₂O₂生产的最新进展,对该领域进行了全面综述,重点关注催化活性部分的设计、制备和机理研究,其中深入讨论了缺陷工程或杂原子掺杂对H₂O₂选择性的增强作用。特别强调了官能团对CMs用于2e-途径的影响。此外,从商业角度出发,强调了用于分散式H₂O₂生产的反应器设计的重要性,弥合了电化学装置中固有催化性能与表观生产率之间的差距。最后,提出了H₂O₂实际电合成的主要挑战和机遇以及未来的研究方向。

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