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Surface hydrogen bonds assisted meso-porous WO3photocatalysts for high selective oxidation of benzylalcohol to benzylaldehyde
Su, Yang1,2; Han, Zhongkang2,3; Zhang, Ling1; Wang, Wenzhong1; Duan, Manyi3; Li, Xiaoman1,2; Zheng, Yali1,2; Wang, Yanggang4; Lei, Xiaoling3
2017
发表期刊Applied Catalysis B: Environmental
ISSN09263373
卷号217页码:108-114
摘要Selective photo–oxidation of alcohols displays high potential in solar energy conversion and reducing environmental pollution, yet its selectivity and conversion in aqueous phase is still far from expectation. Here we report a fluorinated meso-porous WO3photocatalyst (Fm-WO3) exhibits significant selectivity (∼99%) and conversion (∼57%) in transforming benzylalcohol to benzaldehyde in the aqueous solution under the simulated sunlight irradiation. This high reactivity is attributed to the synergistic effect between meso-porous nanostructure and surface fluorination, where meso-porous structure supplies active sites to promote the multi–electron reduction of O2and the surface fluorination assists the transmission of photogenerated holes. First–principles calculations further suggest that surface fluorination brings in an unoccupied impurity state in the band structure of WO3, which exhibits a strong correlation with the hydroxyl group of benzyalcohol and thus bridges the interaction between surfaces and alcohols. Meanwhile, the fluorination promotes the generation of [rad]OH by holes which can be considered as another way to oxidize benzyalcohol. Finally, a generalized reaction mechanism for selective photo-oxidation has been proposed. © 2017 Elsevier B.V.
DOI10.1016/j.apcatb.2017.05.075
EI入藏号20172303731003
EI主题词Hydrogen bonds
EI分类号525.5 Energy Conversion Issues - 657.1 Solar Energy and Phenomena - 801.4 Physical Chemistry - 802.2 Chemical Reactions - 803 Chemical Agents and Basic Industrial Chemicals
引用统计
被引频次:10[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.sic.ac.cn/handle/331005/25934
专题中国科学院上海硅酸盐研究所
通讯作者Zhang, Ling
作者单位1.State Key Laboratory of High Performance Ceramics and Super fine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai; 200050, China;
2.University of Chinese Academy of Sciences, Beijing; 100049, China;
3.Division of Interfacial Water and Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, 2019 JiaLuo Road, Shanghai; 200050, China;
4.Department of Chemistry, Tsinghua University, Beijing; 100084, China
推荐引用方式
GB/T 7714
Su, Yang,Han, Zhongkang,Zhang, Ling,et al. Surface hydrogen bonds assisted meso-porous WO3photocatalysts for high selective oxidation of benzylalcohol to benzylaldehyde[J]. Applied Catalysis B: Environmental,2017,217:108-114.
APA Su, Yang.,Han, Zhongkang.,Zhang, Ling.,Wang, Wenzhong.,Duan, Manyi.,...&Lei, Xiaoling.(2017).Surface hydrogen bonds assisted meso-porous WO3photocatalysts for high selective oxidation of benzylalcohol to benzylaldehyde.Applied Catalysis B: Environmental,217,108-114.
MLA Su, Yang,et al."Surface hydrogen bonds assisted meso-porous WO3photocatalysts for high selective oxidation of benzylalcohol to benzylaldehyde".Applied Catalysis B: Environmental 217(2017):108-114.
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