| Low-temperature catalytic oxidation technology has great application potential in the treatment of volatile organic compounds(VOCs),and manganese oxide has good catalytic performance.This article aims to make up for the shortcomings of cheap,efficient,and long-life non-noble metal catalysts in practical applications,and is dedicated to improving the catalytic oxidation performance of MnO2.Three different modification methods were used to controllably synthesize MnO2 catalysts with special microstructures,and the structure-activity relationship between catalyst structure and catalytic effect was clarified.In-situ DRIFTS technology was used to dynamically track the evolution of reactants,intermediate products and final products,revealing the reaction mechanism of toluene degradation catalyzed by different MnO2 catalysts.This will provide theoretical guidance for the theoretical design of MnO2 catalysts that effectively decompose toluene,and also provide theoretical support for low-temperature catalytic oxidation technology to decompose volatile organic compounds.In this paper,toluene is the target pollutant.Using a fixed bed continuous flow device to evaluate the performance of the catalyst.And using specific crystal plane exposure,vacuum reheat treatment to increase oxygen vacancies,and material reorganization to control MnO2.The MnO2 catalyst was synthesized by a hydrothermal method,and the effects of the exposure of specific crystal planes,oxygen vacancies and the core-shell structure of the MnO2 catalyst on the catalytic degradation of toluene were preliminarily discussed.The detailed research results are as follows:(1)The effect of specific crystal plane exposure on the catalytic degradation of toluene by MnO2.A series ofα-MnO2 catalysts with specific exposed crystal faces of(1 1 0),(2 1 0)and(3 1 0)were prepared by one-step hydrothermal method,respectively.Effects of different exposed crystal planes onα-MnO2 catalytic oxidation of toluene were investigated.Through the combination of experimental characterization and DFT theoretical calculation,the properties and performance of the catalyst were analyzed and explained.Among of them,theα-MnO2 catalyst with(2 1 0)as a specific exposed crystal plane shows the best catalytic performance,and the complete degradation of toluene can be achieved at 140oC.The experimental and characterization results show that the unique atomic arrangement ofα-MnO2-210catalysts enhances charge separation and conversion,promoted the formation of reactive oxygen species and the activation of toluene,which may be the reason whyα-MnO2-210 showed excellent catalytic oxidation performance.(2)The effect of vacuum reheating treatment on the catalytic degradation of toluene byα-MnO2 catalyst.Theα-MnO2 catalyst was prepared by hydrothermal method.The catalyst calcined at 400oC was reheated under vacuum,and the temperature of the vacuum reheat treatment was 140,180,and 200oC,respectively.The catalytic performance of each sample prepared was studied.It can be concluded that theα-MnO2 sample treated at 180oC has the best catalytic performance,and the complete conversion of toluene is achieved at 275oC,which is about 30oC lower than the temperature at whichα-MnO2 without heat treatment completely degrades toluene.The characterization result shows that the reheat treatment under vacuum condition is beneficial to increase the oxygen cavitation on the surface of theα-MnO2 catalyst,thus effectively improving the catalytic performance of theα-MnO2 catalyst.(3)The effect of core-shell structure La MnO3@α-MnO2 composite catalyst on toluene degradation performance.In the process of hydrothermal synthesis ofα-MnO2,0.175,0.35 and 0.525g of La MnO3 were added respectively,to synthesize the core-shell structure La MnO3@α-MnO2 composite catalytic material in situ.The La MnO3@α-MnO2 composite catalyst with complete core-shell structure is obtained when the amount of La MnO3added is 15%;when 10%is added,a semi-closed core-shell structure La MnO3@α-MnO2 can be obtained.The La MnO3@α-MnO2-10 of the semi-enclosed core-shell structure showed the best catalytic activity,the complete conversion of toluene at 225oC.The characterization result shows that a appropriate amount of La MnO3 andα-MnO2 composite material has a core-shell structure,which can increase the content of active oxygen on the surface of theα-MnO2 catalyst,increase the contact interface,and improve its redox capacity,thereby increasing the performance of MnO2 catalyst in the catalytic oxidation of toluene. |