Highly selective oxidation of methane to formaldehyde on tungsten trioxide by lattice oxygen

被引：20

作者：

Fan, Yingying ^{[1
]}

Zhang, Peiyun ^{[1
]}

Lu, Rongxia ^{[1
]}

Jiang, Yuheng ^{[2
,3
]}

Pan, Guoliang ^{[1
]}

Wang, Wei ^{[1
]}

Zhu, Xianglian ^{[1
]}

Wei, Shilei ^{[1
]}

Han, Dongxue ^{[1
]}

Niu, Li ^{[1
]}

机构：

[1] Guangzhou Univ, Ctr Adv Analyt Sci, Analyt & Testing Ctr, Sch Chem & Chem Engn,Guangzhou Key Lab Sensing Ma, Guangzhou 510006, Peoples R China

[2] Chinese Acad Sci, CAS Ctr Excellence Nanosci, Natl Ctr Nanosci & Technol, Key Lab Nanosyst & Hierarchy Fabricat, Beijing 100190, Peoples R China

[3] Peking Univ, Ctr Nanochem, Beijing 100871, Peoples R China

来源：

CATALYSIS COMMUNICATIONS | 2021年 / 161卷

基金：

中国国家自然科学基金;

关键词：

Methane; Photocatalytic; Formaldehyde; Tungsten trioxide; CONVERSION; SURFACE; TIO2; WO3; O-2; ESR;

D O I：

10.1016/j.catcom.2021.106365

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：

Photocatalytic oxidation of methane into formaldehyde in high yield and selectivity remains a grand challenge due to the ineluctable intermediates. Here, we report that a {001}, {010} and {100} facets modified tungsten trioxide photocatalyst enables an intermediate-free oxidation of methane into formaldehyde with 99.4% selectivity. A durable formaldehyde yield of 4.61 mmol g(-1) can be achieved after irradiation for 30 h. Mechanism studies disclose that surface defect and reactive lattice oxygen atom are crucial for the selectivity and productivity promotion. This work provides a valid paradigm for efficient conversion of methane to formaldehyde.

引用

页数：5

共 26 条

[1] Photogenerated-carrier separation along edge dislocation of WO3 single-crystal nanoflower photoanode [J].

Bu, Yuyu ;

Ren, Jun ;

Zhang, Huawei ;

Yang, Dongjiang ;

Chen, Zhuoyuan ;

Ao, Jin-Ping .

JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (18) :8604-8611

[2] Size- and Shape-Controlled Conversion of Tungstate-Based Inorganic-Organic Hybrid Belts to WO3 Nanoplates with High Specific Surface Areas [J].

Chen, Deliang ;

Gao, Lian ;

Yasumori, Atsuo ;

Kuroda, Kazuyuki ;

Sugahara, Yoshiyuki .

SMALL, 2008, 4 (10) :1813-1822

[3] Enhanced Lattice Oxygen Reactivity over Ni-Modified WO3-Based Redox Catalysts for Chemical Looping Partial Oxidation of Methane [J].

Chen, Sai ;

Zeng, Liang ;

Tian, Hao ;

Li, Xinyu ;

Gong, Jinlong .

ACS CATALYSIS, 2017, 7 (05) :3548-3559

[4] Selective photocatalytic oxidation of methane by quantum-sized bismuth vanadate [J].

Fan, Yingying ;

Zhou, Wencai ;

Qiu, Xueying ;

Li, Hongdong ;

Jiang, Yuheng ;

Sun, Zhonghui ;

Han, Dongxue ;

Niu, Li ;

Tang, Zhiyong .

NATURE SUSTAINABILITY, 2021, 4 (06) :509-515

[5] Efficient and selective photocatalytic CH4 conversion to CH3OH with O2 by controlling overoxidation on TiO2 [J].

Feng, Ningdong ;

Lin, Huiwen ;

Song, Hui ;

Yang, Longxiao ;

Tang, Daiming ;

Deng, Feng ;

Ye, Jinhua .

NATURE COMMUNICATIONS, 2021, 12 (01)

[6]

Franz A.W., 2016, Formaldehyde. Ullmann's Encyclopedia of Industrial Chemistry, DOI [DOI 10.1002/14356007.A11619.PUB2, 10.1002/14356007.a11_619.pub2, DOI 10.1002/14356007.A11_619.PUB2]

[7] Porous corundum-type In2O3 nanoflowers: controllable synthesis, enhanced ethanol-sensing properties and response mechanism [J].

Gao, Liping ;

Ren, Fumin ;

Cheng, Zhixuan ;

Zhang, Yuan ;

Xiang, Qun ;

Xu, Jiaqiang .

CRYSTENGCOMM, 2015, 17 (17) :3268-3276

[8] Interaction of molecular oxygen with the vacuum-annealed TiO2(110) surface:: Molecular and dissociative channels [J].

Henderson, MA ;

Epling, WS ;

Perkins, CL ;

Peden, CHF ;

Diebold, U .

JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (25) :5328-5337

[9]

Kim HS, 2017, NAT MATER, V16, P454, DOI [10.1038/NMAT4810, 10.1038/nmat4810]

[10] Electrochemical water oxidation on WO3 surfaces: A density functional theory study [J].

Kishore, Ravi ;

Cao, Xi ;

Zhang, Xueqing ;

Bieberle-Hutter, Anja .

CATALYSIS TODAY, 2019, 321 :94-99

← 1 2 3 →