Defect-rich BN-supported Cu with superior dispersion for ethanol conversion to aldehyde and hydrogen

被引:27
作者
Cheng, Shi-Qun [1 ]
Weng, Xue-Fei [1 ]
Wang, Qing-Nan [1 ]
Zhou, Bai-Chuan [1 ]
Li, Wen-Cui [1 ]
Li, Ming-Run [2 ]
He, Lei [1 ]
Wang, Dong-Qi [1 ]
Lu, An-Hui [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, Liaoning Key Lab Catalyt Convers Carbon Resources, State Key Lab Fine Chem, Dalian 116024, Liaoning, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China
基金
中国国家自然科学基金;
关键词
Ethanol dehydrogenation; Copper; Boron nitride nanosheet; Superior dispersion; In situ DRIFT; BORON-NITRIDE; ACETALDEHYDE ADSORPTION; METHANOL SYNTHESIS; CU/SIO2; CATALYST; DIMETHYL OXALATE; HIGHLY EFFICIENT; INFRARED-SPECTRA; CO ADSORPTION; COPPER; DEHYDROGENATION;
D O I
10.1016/S1872-2067(21)63891-3
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Copper-based heterogeneous catalysts commonly exhibit uncontrolled growth of copper species under reaction conditions because of the low Huttig temperature (surface mobility of atoms) and Tamman temperature (bulk mobility) for copper at just 134 and 405 degrees C, respectively. Herein, we report the use of defect-enriched hexagonal boron nitride nanosheets (BNSs) as a support to anchor the Cu species, which resulted in superior dispersion of the Cu species. The obtained Cu/BNS catalyst was highly stable for ethanol dehydrogenation, with a high selectivity of 98% for producing acetaldehyde and an exceptionally high acetaldehyde productivity of 7.33 g(AcH) g(cat)(-1) h(-1) under a weight hourly space velocity of 9.6 g(EtOH) g(cat)(-1) h(-1). The overall performance of our designed catalyst far exceeded that of most reported heterogeneous catalysts in terms of the stability of the Cu species and the yield of acetaldehyde in this reaction. The hydroxyl groups at the defect edges of BNS were responsible for the stabilization of the copper species, and the metal-support interaction was reinforced through charge transfer, as evidenced by coupling atomic resolution images with probe molecule infrared spectroscopy and X-ray photoelectron spectroscopy. A designed in situ diffuse reflectance infrared Fourier transform spectroscopy study of ethanol/acetaldehyde adsorption further revealed that Cu/BNS favored ethanol adsorption while suppressing acetaldehyde adsorption and further side reactions. This study demonstrates a new method for designing highly dispersed Cu-based catalysts with high durability. (C) 2022, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:1092 / 1100
页数:9
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