Electron-donating N--Ti3+-Ov interfacial sites with high selectivity for the oxidation of primary C-H bonds

被引：12

作者：

Chen, Cheng ^{[1
,2
]}

Wu, Mingge ^{[1
,2
]}

Yang, Chenggong ^{[3
]}

Yu, Xiaolin ^{[4
]}

Yu, Jing ^{[4
]}

Yin, Haibo ^{[5
]}

Li, Ganggang ^{[6
]}

Su, Guijin ^{[1
]}

Hao, Zhengping ^{[6
]}

Song, Maoyong ^{[1
,2
]}

Ma, Chunyan ^{[1
]}

机构：

[1] Chinese Acad Sci, Res Ctr Eco Environm Sci, Key Lab Environm Nanotechnol & Hlth Effects, Beijing 100085, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[3] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

[4] Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Specie, Beijing 100190, Peoples R China

[5] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100084, Peoples R China

[6] Univ Chinese Acad Sci, Res Ctr Environm Mat & Pollut Control Technol, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China

来源：

CELL REPORTS PHYSICAL SCIENCE | 2022年 / 3卷 / 07期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

N-DOPED TIO2; VISIBLE-LIGHT-DRIVEN; OXYGEN VACANCIES; ANATASE TIO2; PHOTOCATALYTIC ACTIVITY; MOLECULAR-OXYGEN; PHASE OXIDATION; BENZOIC-ACID; SOLVENT-FREE; O-2;

D O I：

10.1016/j.xcrp.2022.100936

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Element doping can fabricate different types of oxygen vacancies (O-v) on TiO2, but the effects of O-v coordination and configuration on the oxidation reaction remain unclear. Here, we modify the local geometric ligand environment of Ov by doping N and B into anatase TiO2 (N-TiO2 and B-TiO2). N--Ti3+-Ov is induced in N-TiO2 by substituting O with N, which has similar ionic size and electronega-tivity, and Ti3+-Ov is found in TiO2 and B-TiO2. Density functional theory calculations indicate that N--Ti3+-Ov is more reactive than Ti3+-Ov toward O-2 activation. The resultant N-TiO2-0.25 enriched in N--Ti3+-Ov contributes to a rapid formation of superoxygen spe-cies (dO(2)(-)), which increase the oxidation rate of primary C-H bonds in toluene, and thus exhibits much higher selectivity and yield. The fabrication of N--Ti3+-Ov develops doped catalysts with improved Ov reactivity and enhanced primary C-H bond oxidation selectivity.

引用

页数：17

共 63 条

[1] Electrochemical Performance of Nitrogen-Doped TiO2 Nanotubes as Electrode Material for Supercapacitor and Li-Ion Battery [J].