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Surface Modification of (001) Facets Dominated TiO2 with Ozone for Adsorption and Photocatalytic Degradation of Gaseous Toluene
Yue Yang1, Zhi-yu Wang1, Fan Zhang2, Yi Fan1, Jing-jing Dong1, Song Sun3, Chen Gao*1,4, Jun Bao*1
1.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;2.Beijing Advanced Innovation Center for Big Data and Brain Computing, Beihang University, Beijing 100191, China;3.School of Chemistry and Chemical Engineering, Anhui University, Hefei 230601, China;4.Beijing Advanced Sciences and Innovation center, Chinese Academy of Sciences, Beijing 101407, China
Abstract:
This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated (001) facets for toluene degradation. The performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modi cation, 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 calculation. The surface modi cation with ozone can significantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5c-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 Ti5c-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.
Key words:  Ozone modification, (001) Facets, Toluene degradation, TiO2, In situ diffuse reflectance infrared fourier transform spectroscopy
FundProject:
臭氧修饰(001)晶面TiO2纳米片及其光催化降解甲苯研究
杨 越1,2,3,4, 王徵羽1, 张 帆2, 樊 奕1, 董晶晶1, 孙 松3, 高 琛*1,4, 鲍 骏*1
1.中国科学技术大学国家同步辐射实验室,能源材料化学协同创新中心,安徽省高等学校表面与界面化学与能源催化重点实验室,合肥 230029;2.北京航空航天大学北京大数据与脑计算高级创新中心,北京 100191;3.安徽大学化学化工学院,合肥 230601;4.中国科学院北京高等科学与创新中心,北京 101407
摘要:
本文系统研究了臭氧修饰对(001)主导晶面锐钛矿型TiO2光催化剂降解甲苯性能的影响. 利用自行搭建的光催化VOCs降解装置对催化剂光降解甲苯的性能进行了测试. 通过多种表征手段,结合原位DRIFTS和DFT计算研究了臭氧表面修饰及甲苯吸附和降解机理. 结果表明,用臭氧进行表面修饰可以显著提高(001)主导晶面TiO2光催化降解甲苯的性能. (001)晶面上丰富的5c-Ti不饱和配位是臭氧分子的吸附位点,其解离后形成的Ti-O键与H2O分子结合,在表面生成大量孤立的Ti5c-OH. Ti5c-OH 是甲苯分子的吸附位,它的形成显著提高了对甲苯分子的吸附能力. 在光照下Ti5c-OH与光生空穴结合能形成·OH自由基. 通过臭氧解离产生的O2也可以与光生电子结合形成超氧自由基. 这些具有强氧化性活性自由基的形成促进了对气相甲苯的光催化降解速率.
关键词:  臭氧修饰,(001)晶面,甲苯降解,TiO2,原位DRIFTS
DOI:10.1063/1674-0068/cjcp1903062
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