期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 581, 期 -, 页码 719-728出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2020.07.140
关键词
Bi2MoO6; Amine coupling; Visible light; Photocatalysis; Charge carrier lifetime
资金
- Science Achievement Scholarship of Thailand
- Murata Science Foundation, Japan
- Chiang Mai University, Thailand
- Office of Commission on Higher Education (OHEC)
- Thailand Research Fund [DBG6280005]
- Basic Research Fund through Center of Excellence in Materials Science and Technology
- Center of Excellence for Innovation in Chemistry (PERCH-CIC), Ministry of Higher Education, Science, Research and Innovation
Bismuth molybdate nanocatalysts with oxygen vacancies significantly enhance the photocatalytic performance for the oxidative coupling of benzylamine to N-benzylidenebenzylamine under visible light irradiation. The oxygen-deficient Bi2MoO6 nanoplatelets exhibit higher catalytic activity due to their high surface-to-volume ratio and oxygen vacancies.
Herein, bismuth molybdate (Bi2MoO6) nanocatalysts containing oxygen vacancies (OVs) are found to considerably promote the photocatalytic performance toward oxidative coupling of benzylamine to N-benzylidenebenzylamine under visible light irradiation. The structure-activity relationship for this interesting catalyst is revealed for the first time. The oxygen-deficient Bi2MoO6 nanoplatelets (BMO-NPs) are synthesized using ethylene glycol-ethanol solvent mixture as a reaction medium in solvothermal method. A comparison with hydrothermally prepared Bi2MoO6 square-like sheets (BMO-SHs) suggests that the nanoplatelets are much smaller in size and contain higher amount of OVs. Benzylamine conversion over the BMO-NPs is ca. 4.0 times higher than that over the BMO-SHs and ca. 3.8 and ca. 34.6 times higher than that over the commercial benchmark TiO(2 )P25 and BiVO4 catalysts, respectively. The BMO-NPs achieve more than 80% product yield within 2 h of irradiation regardless of substituents of benzylamine derivatives. The enhanced activity of BMO-NPs is due to synergistic roles of high surface-to-volume ratio and OVs, providing enlarged active area, extended light absorption range and improved charge separation and transfer efficiency as evidenced from UV-vis DRS, BET surface area, photocurrent response, electrochemical impedance spectroscopy, and time-resolved fluorescence decay measurements. EPR-trapping and radical scavenging experiments indicate O-2(center dot) as a main active species rather than O-1(2) and a plausible imine formation mechanism via O-2(center dot)-assisted charge transfer is proposed accordingly. The work offers an alternative facile preparation method to design efficient semiconductor photocatalysts and for the first time reveals a possible benzylamine coupling mechanism over the oxygen-deficient Bi2MoO6 nanocatalyst. (C) 2020 Elsevier Inc. All rights reserved.
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