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负载铂单原子的氧化锰光热协同催化增强甲苯氧化

Enhanced toluene oxidation by photothermal synergetic catalysis on manganese oxide embedded with Pt single-atoms.

作者信息

Wang Yang, Dai Jinyu, Wang Min, Qi Fenggang, Jin Xixiong, Zhang Lingxia

机构信息

State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding-xi Road, Shanghai 200050, PR China; Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing 100049, PR China.

State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding-xi Road, Shanghai 200050, PR China.

出版信息

J Colloid Interface Sci. 2023 Apr 15;636:577-587. doi: 10.1016/j.jcis.2023.01.053. Epub 2023 Jan 14.

Abstract

The degradation of volatile organic compounds (VOCs) at low temperature remains a big challenge. Photothermal catalysis coupling the advantages of photocatalysis and thermocatalysis is promising to address this issue. However, there is still a long way to construct highly active catalysts and deeply understand the mechanism of photothermal catalysis. Herein, maganese oxide (MnO)catalysts embedded with Pt single-atoms (0.11 wt% Pt) have achieved greatly enhanced toluene conversion of 95%, far surpassing most supported Pt photothermal catalysts. The excellent catalytic activity has been disclosed to derive from the synergetic effect oflight-driven thermocatalysis and photocatalysis. The light-driven thermocatalysis predominates and the strong electron transfer from Pt single-atoms to MnO improves the activity of surface lattice oxygen to boost the generation of benzoic acid and the mineralization of toluene. Meanwhile, in photocatalytic process, Pt single-atoms accelerate the generation of superoxide radicals (O), which facilitate the ring-opening and deep oxidation of toluene. This understanding on the photothermal synergetic mechanism will inspire the design of highly efficient catalysts for VOCs oxidation.

摘要

低温下挥发性有机化合物(VOCs)的降解仍然是一个巨大的挑战。光热催化结合了光催化和热催化的优点,有望解决这一问题。然而,构建高活性催化剂并深入理解光热催化的机理仍有很长的路要走。在此,嵌入0.11 wt%铂单原子的氧化锰(MnO)催化剂实现了甲苯转化率大幅提高至95%,远远超过了大多数负载型铂光热催化剂。已揭示出这种优异的催化活性源于光驱动热催化和光催化的协同效应。光驱动热催化起主导作用,铂单原子向MnO的强电子转移提高了表面晶格氧的活性,促进了苯甲酸的生成和甲苯的矿化。同时,在光催化过程中,铂单原子加速了超氧自由基(O)的生成,这有利于甲苯的开环和深度氧化。对光热协同机理的这种理解将激发用于VOCs氧化的高效催化剂的设计。

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