Oxygen vacancies induced special CO2 adsorption modes on Bi2MoO6 for highly selective conversion to CH4

被引：285

作者：

Yang, Xianglong ^{[1
]}

Wang, Shengyao ^{[1
,2
]}

Yang, Nan ^{[1
]}

Zhou, Wei ^{[3
]}

Wang, Pei ^{[1
]}

Jiang, Kai ^{[1
]}

Li, Shu ^{[1
]}

Song, Hui ^{[2
,4
]}

Ding, Xing ^{[1
]}

Chen, Hao ^{[1
]}

Ye, Jinhua ^{[2
,4
,5
]}

机构：

[1] Huazhong Agr Univ, Minist Educ, Key Lab Environm Correlat Dietol, Coll Sci, Wuhan 430070, Hubei, Peoples R China

[2] NIMS, Int Ctr Mat Nanoarchitecton WPI MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050055, Japan

[3] Tianjin Univ, Sch Mat Sci & Engn, TJU NIMS Int Collaborat Lab, Tianjin 300072, Peoples R China

[4] Hokkaido Univ, Grad Sch Chem Sci & Engn, Sapporo, Hokkaido 0600814, Japan

[5] Sch Mat Sci & Engn, TU NIMS Joint Res Ctr, Tianjin 300072, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2019年 / 259卷

基金：

中国国家自然科学基金;

关键词：

CO2; photoreduction; Oxygen vacancy; Selectivity; Bi2MoO6; LIGHT-DRIVEN CO2; PHOTOCATALYTIC REDUCTION; EXCITON DISSOCIATION; CARBON-DIOXIDE; SURFACE; TIO2; ANATASE; ABSORPTION; NANOSHEETS; BIOBR;

D O I：

10.1016/j.apcatb.2019.118088

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：

Search for suitable photocatalysts with ultrahigh selective generation of CH4 from CO2 is a great challenge in artificial photocatalysis. Herein, effective CO2 photoconversion to CH4 with high selectivity up to 96.7% is achieved over oxygen-deficient Bi-2 MoO6 under visible-light. Various characterizations and DFT calculations indicated that well-designed oxygen vacancies (OVs) on the {001} surface of Bi2MoO6 can not only enhance light harvesting and e(-)/h(+) separation, but favor CO2 adsorption in a special bidentate carbonate mode, which thermodynamically supports the further hydrogenation of intermediate *CO to generate CH4. Based on the in-situ infrared spectroscopy analysis, the CO2 adsorption modes and reaction intermediates of two pathways over Bi2MoO6 with or without OVs were figured out. The reasonable photocatalytic mechanism for highly selective conversion to CH4 was also proposed. This work provides new insights to the role of OVs in selective CO2 photoconversion, and paves ways to design efficient CH4 evolution systems.

引用

页数：8

共 53 条

[1] Cu2O/TiO2 heterostructures for CO2 reduction through a direct Z-scheme: Protecting Cu2O from photocorrosion [J].