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Continuous generation of lattice oxygen via redox engineering for boosting toluene degradation performances

Chinese Journal of Chemical Engineering 2021年第6期34卷 258-266页

作者： Shiya He Zhimin You Xin Jin Yi Wu Cheng Chen He Zhao Jian Shen Department of Environment and Resources Xiangtan UniversityXiangtan 411105China State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringChina University of PetroleumQingdao 266580China Beijing Engineering Research Center of Process Pollution Control Division of Environment Technology and EngineeringKey Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Excellent performances promoted by lattice oxygen have attracted wide attention for catalytic degradation of volatile organic compounds(VOCs).However,how to control the continuous regeneration of lattice oxygen from the support is seldom *** this study,we selected sepiolite supported manganese-cobalt oxides(Co_(x)Mn_(100-x)O_(y))as model catalysts by tuning Co/(Co+Mn)mass ratio(x=3%,10%,15%,and 20%)to enhance toluene degradation efficiency,owing to lattice oxygen regeneration by redox cycle existing at the interface and Mn species with high valence state,initiated by cobalt catalytic performance under the role of crystal field stability *** results of activity test show that the sepiolite-Co_(15)Mn_(85)O_(y)catalyst exhibit outperformances at 193℃with 10,000 h^(-1)*** addition,the catalyst existed at the bottom of the"volcano"curve correlated T_(50)or T_(90)with Co/(Co+Mn)weight ratio is sepiolite-Co_(15)Mn_(85)O_(y),conforming its *** characterized by investigating active sites structural and electronic properties,the essential of superior catalytic activity is attributed to the grands of lattice oxygen continuous formation resulted from redox engineering based on the high atomic ratio of surface lattice oxygen with continuous refilled from the support and that of Mn^(4+)/Mn^(3+)cycle initiated by cobalt catalytic *** in all,redox engineering,not only promotes grands of active species reversible regeneration,but supplies an alternative catalyst design strategy towards the terrific efficiency-to-cost ratio performance.

关键词： Redox engineering Crystal field stability phase Lattice oxygen toluene degradation

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Defect-poor BaSn(OH)6 enhanced charge separation for efficient photocatalytic degradation of toluene

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Journal of Environmental Sciences 2023年第12期134卷 86-95页

作者： Xuemei Wang Xi Zhou Ruiben Jin Tianqi Tan Hao Ma Ruimei Fang Bangwei Deng Fan Dong College of Environment and Resources Chongqing Key Laboratory of Catalysis and New Environmental MaterialsChongqing Technology and Business UniversityChongqing 400067China Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313001China Hangzhou Tianliang Detection Technology COM. LTD.Hangzhou 311202China

Crystal defect is well-known to have a significant effect on the photocatalytic performance of semiconductors. Herein, defect-rich and-poor BaSn(OH)6(BSOH-Sn and BSOH-Ba) photocatalysts were synthesized by exchanging the addition order of Ba and Sn. Results show that the defect-poor BSOH-Ba exhibited more efficient toluene degradation under ultraviolet(UV) light, which could attribute to the great suppression of photogenerated electron-hole(e--h+) pairs recombination by tuning the defect concentration. The low defect concentration in BSOH-Ba finally promotes the charge separation efficiency, the generation of reactive oxygen species(ROS), and the photocatalytic toluene degradation reactions. This work not only provides an effective way to inhibit the recombination of photogenerated carriers and improve the photocatalytic performance, but also promotes the understanding of defective perovskite-type hydroxide for more photoreactions.

关键词： Defect Charge recombination BaSn(OH)6 toluene degradation Photocatalysis

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Surface Modification of (001) Facets Dominated TiO2 with Ozone for Adsorption and Photocatalytic degradation of Gaseous toluene

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Chinese Journal of Chemical Physics 2019年第5期32卷 611-619页

作者： Yue Yang Zhi-yu Wang Fan Zhang Yi Fan Jing-jing Dong Song Sun Chen Gao Jun Bao National Synchrotron Radiation Laboratory Collaborative Innovation Center of Chemistry for Energy Materials Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes University of Science and Technology of China Hefei 230029 China Beijing Advanced Innovation Center for Big Data and Brain Computing Beihang University Beijing 100191 China School of Chemistry and Chemical Engineering Anhui University Hefei 230601 China Beijing Advanced Sciences and Innovation center Chinese Academy of Sciences Beijing 101407 China

This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated（001） facets for toluene *** performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mechanism were established by a combination of various characterization methods, in situ diffuse reflectance infrared fourier transform spectroscopy, and density functional theory *** surface modification with ozone can significantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5 c-Ti sites on（001）facets act as the adsorption sites for ozone. The formed Ti–O bonds reacted with H2O to generate a large amount of isolated Ti5 c-OH which act as the adsorption sites for toluene,and thus significantly increase the adsorption capacity for toluene. The outstanding photocatalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH·radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.

关键词： Ozone modification (001) Facets toluene degradation TiO2 In situ diffuse reflectance infrared fourier transform spectroscopy

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Accelerated oxidation of VOCs via vacuum ultraviolet photolysis coupled with wet scrubbing process

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Journal of Environmental Sciences 2023年第12期134卷 55-64页

作者： Ruijie Xie Dongxue Lei Xiaowen Xie Ziyi Suo Dennis Y.C.Leung Jianping Cao Fang Ruimei Haibao Huang School of Environmental Science and Engineering Sun Yat-sen UniversityGuangzhou 510275China Department of Mechanical Engineering University of Hong KongHong Kong 999077China College of Environment and Resources Chongqing Technology and Business UniversityChongqing 400067China Scientific Research Academy of GuangXi Environmental Protection Nanning 530022China

Vacuum ultraviolet(VUV) photolysis is a facile method for volatile organic compounds(VOCs) elimination, but is greatly limited by the relatively low removal efficiency and the possible secondary pollution. To overcome above drawbacks, we developed an efficient method for VOCs elimination via VUV photolysis coupled with wet scrubbing process. In this coupled process, volatile toluene, a representative of VOCs, was oxidized by the gas-phase VUV photolysis, and then scrubbed into water for further oxidation by the liquid-phase VUV photolysis. More than 96% of toluene was efficiently removed by this coupled process, which was 2 times higher than that in the gas-phase VUV photolysis. This improvement was attributed to the synergistic effect between gas-phase and liquid-phase VUV photolysis. O3and HO·are the predomination reactive species for the toluene degradation in this coupled process, and the generation of O3in gas-phase VUV photolysis can efficiently enhance the HO·production in liquid-phase VUV photolysis. The result from in-situ proton transfer reaction ionization with mass analyzer(PTR-MS) further suggested that most intermediates were trapped by the wet scrubbing process and efficiently oxidized by the liquid-phase VUV photolysis, showing a high performance for controlling the secondary pollution. Furthermore, the result of stability test and the reuse of solution demonstrated that this coupled process has a highly stable and sustainable performance for toluene degradation. This study presents an environmentally benign and highly efficient VUV photolysis for gaseous VOCs removal in the wet scrubbing process.

关键词： Volatile organic compounds(VOCs) Vacuum ultraviolet(VUV)photolysis Wet scrubbing process toluene degradation Intermediates analysis

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Rational Design of LDH/Zn_(2)SnO_(4) Heterostructures for Efficient Mineralization of toluene Through Boosted Interfacial Charge Separation

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Energy & Environmental Materials 2023年第1期6卷 317-324页

作者： Ben Lei Wen Cui Peng Chen Ruimin Chen Yanjuan Sun Ki-Hyun Kim Fan Dong Research Center for Environmental and Energy Catalysis Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China College of Resources and Environmental Engineering Guizhou UniversityGuiyang 550025China Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313001China School of Resources and Environment University of Electronic Science and Technology of ChinaChengdu 611731China Department of Civil and Environmental Engineering Hanyang University222 Wangsimni-RoSeoul 04763Korea State Centre for International Cooperation on Designer Low carbon and Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China

It is crucial to efficiently separate and transport photo-induced charge carriers for the effective implementation of photocatalysis toward environmental remediation.A rational design strategy is proposed to validate such proposition through the construction of an interfacial structure in the form of LDH/Zn_(2)SnO_(4) heterostructures in this *** interfacial charge transfer on LDH/Zn_(2)SnO_(4) is greatly promoted via the unique charge transfer pathway,as characterized by transient photocurrent responses,X-ray photoelectron spectroscopy,electron paramagnetic resonance spectrum,and photoluminescence *** such,it contributes to the generation of reactive oxygen species(ROS)and the activation of reactants for the mineralization of *** to the in situ DRIFTS spectra analysis,the accumulation of benzoic acid takes place possibly through the partial oxidation of the methyl group on toluene at the interface of the LDH/Zn 2 SnO 4 *** process can greatly promote the photocatalytic oxidation of toluene with the enhanced ring-opening *** LDH/Zn 2 SnO 4 is thus demonstrated as superior photocatalyst against toluene(removal efficiency of 89.5%;mineralization of 83.1%;and quantum efficiency of 4.55×10^(−6) molecules/photon).As such,the performance of this composite far exceeds that of their individual components(e.g.,P25,pure Mg-Al LDH,or Zn_(2)SnO_(4)).This study is expected to offer a new path to the interfacial charge transfer mechanism based on the design of highly efficient photocatalysts for air purification.

关键词： heterostructure interfacial charge transfer photocatalysis toluene degradation

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Efficient activation of the Co/SBA-15catalyst by high-frequency AC-DBD plasma thermal effects for toluene removal

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Plasma Science and Technology 2024年第8期26卷 84-94页

作者：李越姜楠刘政妍秦亮彭邦发王荣刚孙玉荣李杰 School of Environment Dalian University of TechnologyDalian 116024People’s Republic of China School of Electrical Engineering Dalian University of TechnologyDalian 116024People’s Republic of China College of Electrical and Power Engineering Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China Canmax Technologies Co. Ltd.Suzhou 215121People’s Republic of China

Dielectric barrier discharge(DBD)plasma excited by a high-frequency alternating-current(AC)power supply is widely employed for the degradation of volatile organic compounds(VOCs).However,the thermal effect generated during the discharge process leads to energy waste and low energy utilization *** this work,an innovative DBD thermally-conducted catalysis(DBD-TCC)system,integrating high-frequency AC-DBD plasma and its generated thermal effects to activate the Co/SBA-15 catalyst,was employed for toluene ***,Co/SBA-15 catalysts are closely positioned to the ground electrode of the plasma zone and can be heated and activated by the thermal effect when the voltage exceeds 10 k ***12.4 k V,the temperature in the catalyst zone reached 261℃ in the DBD-TCC system,resulting in an increase in toluene degradation efficiency of 17%,CO_(2)selectivity of 21.2%,and energy efficiency of 27%,respectively,compared to the DBD system *** contrast,the DBD thermally-unconducted catalysis(DBD-TUC)system fails to enhance toluene degradation due to insufficient heat absorption and catalytic activation,highlighting the crucial role of AC-DBD generated heat in the activation of the ***,the degradation pathway and mechanism of toluene in the DBD-TCC system were *** work is expected to provide an energy-efficient approach for high-frequency AC-DBD plasma removal of VOCs.

关键词： high-frequency alternating-current power thermal effect dielectric barrier discharge toluene degradation Co/SBA-15 catalysts

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