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氧化镁铝尖晶石诱导形成具有稳定致密界面的氧化物异质结用于高效电合成过氧化氢

Oxide heterojunction with stable and dense interface induced by magnesium aluminum oxide spinel for high-efficiency electrosynthesis of hydrogen peroxide.

作者信息

Wu Suqin, Pu Chen, Deng Daijie, Xu Li, Wu Jianchun, Yan Cheng, Li Henan

机构信息

School of Chemistry and Chemical Engineering, Institute for Energy Research, Institute of Quantum and Sustainable Technology of Jiangsu University, Jiangsu University, Zhenjiang 212013, China.

School of Chemistry and Chemical Engineering, Institute for Energy Research, Institute of Quantum and Sustainable Technology of Jiangsu University, Jiangsu University, Zhenjiang 212013, China; School of Mechanical, Medical and Process Engineering, Queensland University of Technology (QUT), Brisbane, Queensland 4001, Australia.

出版信息

J Colloid Interface Sci. 2025 Oct 15;696:137848. doi: 10.1016/j.jcis.2025.137848. Epub 2025 May 10.

Abstract

Two-electron oxygen reduction reaction (2e ORR) is a low cost and high security method for the electrosynthesis of hydrogen peroxide (HO). Nevertheless, the 2e ORR selectivity and activity are difficult to control. Herein, a MgAlO/CoO heterojunction electrocatalyst has been successfully synthesized by the calcination of layered double hydroxide (LDH). As a 2e ORR electrocatalyst, the MgAlO/CoO demonstrates a high HO selectivity of 90 % with excellent stability. In a flow cell, the MgAlO/CoO electrocatalyst exhibits a HO yield of 10.2 mol g h and a faradaic efficiency of 85 %. Experimental results reveal that the MgAlO spinel is conducive to the high dispersion of metal and stable structure of catalyst. The stable and dense heterojunction interface can be induced by the MgAlO spinel in the MgAlO/CoO, ultimately leading to the high activity and stability of catalyst. Density functional theory (DFT) calculations uncover that the construction of MgAlO/CoO can facilitate charge transfer and adjust the electronic structure, thereby promoting the 2e ORR selectivity for high-efficiency HO production. Additionally, the HO generated by the MgAlO/CoO electrocatalyst can achieve in-situ degradation of rhodamine B. The possible degradation pathway is also proposed. This strategy provides a reasonable way to prepare 2e ORR electrocatalysts for HO production toward pollutant degradation.

摘要

双电子氧还原反应(2e ORR)是一种用于电合成过氧化氢(HO)的低成本、高安全性方法。然而,2e ORR的选择性和活性难以控制。在此,通过层状双氢氧化物(LDH)的煅烧成功合成了MgAlO/CoO异质结电催化剂。作为一种2e ORR电催化剂,MgAlO/CoO表现出90%的高HO选择性和出色的稳定性。在流动池中,MgAlO/CoO电催化剂的HO产率为10.2 mol g h,法拉第效率为85%。实验结果表明,MgAlO尖晶石有利于金属的高度分散和催化剂结构的稳定。MgAlO/CoO中的MgAlO尖晶石可诱导形成稳定且致密的异质结界面,最终导致催化剂具有高活性和稳定性。密度泛函理论(DFT)计算表明,MgAlO/CoO的构建可促进电荷转移并调整电子结构,从而提高2e ORR选择性以高效生产HO。此外,MgAlO/CoO电催化剂产生的HO可实现罗丹明B的原位降解,并提出了可能的降解途径。该策略为制备用于HO生产以降解污染物的2e ORR电催化剂提供了一种合理的方法。

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