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SrSbO 上的表面晶格氧活化增强甲苯的光催化矿化:从反应物活化、中间体转化到产物脱附

Surface Lattice Oxygen Activation on SrSbO Enhances the Photocatalytic Mineralization of Toluene: from Reactant Activation, Intermediate Conversion to Product Desorption.

作者信息

Chen Lvcun, Chen Peng, Wang Hong, Cui Wen, Sheng Jianping, Li Jieyuan, Zhang Yuxin, Zhou Ying, Dong Fan

机构信息

The Center of New Energy Materials and Technology, School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, P. R. China.

Yangtze Delta Region Institute (Huzhou), & Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Huzhou 313001, China.

出版信息

ACS Appl Mater Interfaces. 2021 Feb 3;13(4):5153-5164. doi: 10.1021/acsami.0c20996. Epub 2021 Jan 21.

Abstract

Transition-metal oxide photocatalysis has attracted increasing attention in environmental remediation and solar energy conversion. Surface lattice oxygen is the key active site on the metal oxide, but its role and activation mechanism in the photocatalytic VOC mineralization are still unclear. In this work, we have demonstrated that SrSbO exhibits an excellent photocatalytic activity and stability compared to TiO (P25) in gaseous toluene mineralization because the lattice oxygen on SrSbO can be activated efficiently. The lattice oxygen of SrSbO promotes the adsorption and activation of O and HO molecules and enhances the production of O and OH radicals, as confirmed by the electron spin resonance and DFT calculations. The in situ diffuse reflectance infrared Fourier transform spectroscopy spectra are applied to dynamically monitor the intermediate activation and selective conversion. Combined with DFT calculation, the role and the mechanism of lattice oxygen in photocatalysis have been revealed. Owing to the promoted surface lattice oxygen, the selectivity for benzoic acid formation is enhanced and final product desorption is promoted, which could largely advance the ring opening and mineralization of toluene. This work reveals the origin of lattice oxygen activation and the role for efficient VOC degradation at the atomic scale.

摘要

过渡金属氧化物光催化在环境修复和太阳能转换方面已引起越来越多的关注。表面晶格氧是金属氧化物上的关键活性位点,但其在光催化挥发性有机化合物矿化中的作用和活化机制仍不清楚。在这项工作中,我们已经证明,与TiO(P25)相比,SrSbO在气态甲苯矿化中表现出优异的光催化活性和稳定性,因为SrSbO上的晶格氧可以被有效活化。电子自旋共振和密度泛函理论计算证实,SrSbO的晶格氧促进了O和HO分子的吸附和活化,并增强了O和OH自由基的产生。原位漫反射红外傅里叶变换光谱用于动态监测中间产物的活化和选择性转化。结合密度泛函理论计算,揭示了晶格氧在光催化中的作用和机制。由于表面晶格氧的促进作用,苯甲酸生成的选择性增强,最终产物的脱附得到促进,这在很大程度上促进了甲苯的开环和矿化。这项工作揭示了晶格氧活化的起源以及在原子尺度上高效降解挥发性有机化合物的作用。

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