Visible light driven selective oxidation of amines to imines with BiOCl: Does oxygen vacancy concentration matter?

Mao, Chengliang1; Cheng, Honggang1; Tian, Hao2; Li, Hao1; Xiao, Wen-Jing1; Xu, Hu2; Zhao, Jincai1; Zhang, Lizhi1

2018-07-15

10.1016/j.apcatb.2018.01.018

APPLIED CATALYSIS B-ENVIRONMENTAL   影响因子和分区

0926-3373

1873-3883

The relationship between oxygen vacancy (OV) concentration of semiconductors and their photocatalytic performances is far from clarified. In this study, by tuning the OV concentration of BiOCl (001) surface via a novel H2O2 treatment coupled infrared irradiation method, we demonstrate that OV concentration of BiOCl (001) surface strongly determine its surface atomic and electronic structures to modulate the photocatalytic pathways. Being of shorter Bi-Bi and Bi-O bond lengths as well as more electrons being less localized, BiOCl (001) surface with higher OV concentration favored molecular oxygen activation to generate O-2(2-) via a two-electron transfer pathway, while the generated O-2(2-) could prevent the over oxidation of amines and thus achieve high selectivity in the oxidation of amines to imines. Similar phenomena were also observed for other semiconductor photo catalysts such as TiO2 and Nb2O5, suggesting the generality of oxygen vacancy concentration mediated selectivity enhancement. These findings shed light on the relationship between the oxygen vacancy concentration and the surface structure of semiconductor photocatalysts and offer a novel pathway to realize photocatalytic selective oxidation of amines to imines.

Oxygen vacancies Molecular oxygen activation Bismuth oxychloride Selective amines oxidation Photocatalysis

SCI ; EI

英语

ESI高被引

其他

Graduate Education Innovation Funding Project Grant from CCNU[2016CXZZ54]

Chemistry ; Engineering

Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical

WOS:000427663900010

ELSEVIER SCIENCE BV

20180604772842

Amines ; Bismuth compounds ; Chemical activation ; Chlorine compounds ; Electronic structure ; Light ; Magnetic semiconductors ; Molecular oxygen ; Niobium oxide ; Oxidation ; Photocatalysis ; Titanium dioxide ; Vacancies

Magnetic Materials:708.4 ; Light/Optics:741.1 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Crystalline Solids:933.1

CHEMISTRY

Web of Science

1.Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China
2.South Univ Sci & Technol China, Dept Phys, Shenzhen 518055, Peoples R China

Mao, Chengliang,Cheng, Honggang,Tian, Hao,et al. Visible light driven selective oxidation of amines to imines with BiOCl: Does oxygen vacancy concentration matter?[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2018,228:87-96.

Mao, Chengliang.,Cheng, Honggang.,Tian, Hao.,Li, Hao.,Xiao, Wen-Jing.,...&Zhang, Lizhi.(2018).Visible light driven selective oxidation of amines to imines with BiOCl: Does oxygen vacancy concentration matter?.APPLIED CATALYSIS B-ENVIRONMENTAL,228,87-96.

Mao, Chengliang,et al."Visible light driven selective oxidation of amines to imines with BiOCl: Does oxygen vacancy concentration matter?".APPLIED CATALYSIS B-ENVIRONMENTAL 228(2018):87-96.