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Undervalued role of metal-carbon junction in selective generation of H2O2: An example of the zinc-carbon junction edge providing asymmetric active sites for efficient oxygen reduction

Journal 2024 · IF 13.3 · 发表于 2024 年 10 月 21 日
作者: Chengyu Duan,Yinglong Lu,Zheshun Ou,Mengdi Sun,Guanghui Luo,Huimin Liu,Ruilin Wang,Yijie Wang,Zhuofeng Hu
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摘要

The spontaneous oxygen reduction is a potential technology for in-situ H 2 O 2 production, which gets rid of the dependence on electricity and solar energy. Previous some metal–carbon compounds reported are feasible to trigger oxygen reduction. These reports always claim the high H 2 O 2 generation ability of metal–carbon composites, while rarely discuss the contribution of carbon and the carbon–metal junction to the oxygen reduction process. Inspired by the dual active sites, we infer that the role of interfacial carbon in metal–carbon composites is underestimated. By a heat treatment of the co-precipitate of zinc and glucose, the Zn-C junction is constructed in Zn-gc to achieve a spontaneous selective reduction of O 2 to H 2 O 2 . The Zn-C interface edge is active site, where an asymmetric activation is achieved by bonding two O atoms from O 2 to C and Zn, respectively. The Zn traction to one of the O atoms is mainly in xy plane, while the C traction to the other O atom is parallel to z-axis. The yield of H 2 O 2 produced per gram of Zn increases from 27.89 mg to 122.21 mg, an improvement of 4.38 times. And the inertness of Zn and its oxygen-containing compounds towards H 2 O 2 enables Zn-gc/O 2 system to stabilize H 2 O 2 over a long period of time. This work reveals the crucial role of neglected junction interfaces in oxygen reduction reactions in metal–carbon composites.

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