Water-Mediated Photocatalytic Coproduction of Diesel Fuel Additives and Hydrogen from Dimethyl Ether

被引:0
|
作者
Liu, Shiyang [1 ,2 ]
Huang, Yike [3 ]
Luo, Nengchao [1 ]
Zhang, Jian [1 ]
Qiao, Botao [4 ]
Wang, Feng [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] AI Sci Inst, Beijing 100080, Peoples R China
[4] Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
photocatalysis; dimethyl ether; diesel fuel; H-2; hole transfer; OXIDATION; NANOPARTICLES; PERFORMANCE; INTERFACE; DYNAMICS; ZEOLITE; SURFACE; SITES; HOLES;
D O I
10.1021/acscatal.4c01132
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
Dimethyl ether (DME) coupling via prior C-H bond scission affords H-2 and long-chain oxygenates that can be used as diesel fuel additives. However, the C-H bond of DME is recalcitrant, requiring activation by oxidants for subsequent C-C bond coupling, and overoxidation to CO2 by nonselective oxidants is inevitable. Here, by establishing a channel for hole transfer from the Pt/TiO2 photocatalyst to DME, the C-H bond of DME is broken, affording H-2 and diesel fuel additives consisting of glycol dimethyl ether (GDE) and oligomers. Adsorbed water on Pt/TiO2 fosters hole transfer by forming hydrogen bonds with both Pt/TiO2 surface and DME. Because of the hydrogen bonding, photogenerated holes are extracted from Pt/TiO2 by water and eventually transferred to DME. As a result, the productivities of the diesel fuel and H-2 are increased by 8.7 and 12.4 folds, respectively. This work provides a route to produce two kinds of fuels from an abundant feedstock.
引用
收藏
页码:6807 / 6815
页数:9
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