Crystal-plane effects of anatase TiO2 on the selective hydrogenation of crotonaldehyde over Ir/TiO2 catalysts

被引:35
作者
Jia, Aiping [1 ,2 ,3 ]
Zhang, Yunshang [1 ,2 ]
Song, Tongyang [4 ]
Zhang, Zhenhua [3 ]
Tang, Cen [3 ]
Hu, Yiming [3 ]
Zheng, Wanbin [3 ]
Luo, Mengfei [3 ]
Lu, Jiqing [3 ]
Huang, Weixin [1 ,2 ,5 ]
机构
[1] Univ Sci & Technol China, CAS Key Lab Mat Energy Convers, Hefei Natl Lab Phys Sci Microscale,Anhui Higher E, Key Lab Surface & Interface Chem & Energy Catalys, Hefei 230026, Peoples R China
[2] Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China
[3] Zhejiang Normal Univ, Inst Phys Chem, Minist Educ Adv Catalysis Mat, Key Lab, Jinhua 321004, Zhejiang, Peoples R China
[4] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
[5] Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
Hydrogenation; alpha; beta - unsaturated aldehyde; Ir/TiO2; Crystal plane effect; Defects; Reaction mechanism; GENERATION VIBRATIONAL SPECTROSCOPY; METAL-SUPPORT INTERACTIONS; ALPHA; BETA-UNSATURATED ALDEHYDES; TITANIUM OXIDE; PERFORMANCE; ADSORPTION; IRIDIUM; FACETS; SITES; C=O;
D O I
10.1016/j.jcat.2020.12.012
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Supported Ir/TiO2 catalysts with the anatase TiO2 nanocrystals exposing {101}, {100} and {001} planes were tested for selective hydrogenation of crotonaldehyde. The Ir/TiO2-{101} catalyst dominantly exposing {101} plane gave a initial reaction rate of 166.1 mu mol g(Ir)(-1) s (1) at 80 degrees C and a turnover frequency of crotyl alcohol formation of 0.022 s (1), which is 5 and 7 times respectively higher than those obtained on the Ir/TiO2-{001} catalyst dominantly exposing {001} plane even though they have similar Ir particle sizes (ca. 1.3 nm). The reaction behaviors were related to the surface oxygen vacancy, which served as surface acid sites and provide adsorption sites for C=O bond in the CRAL molecule. Therefore, the higher concentration of oxygen vacancy in the Ir/TiO2-{101} accounted for the improved performance compared to the Ir/TiO2-{001}. However, strong adsorption of crotonaldehyde and/or products on the catalyst surface, as well as the CO poisoning via decarbonylation of crotonaldehyde, were the main reasons for the catalyst deactivation. (C) 2020 Elsevier Inc. All rights reserved.
引用
收藏
页码:10 / 22
页数:13
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