Effect of Calcination Temperature on the Textural Properties and Catalytic Behavior of the Al 2 O 3 Doped Mesoporous Mon
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Effect of Calcination Temperature on the Textural Properties and Catalytic Behavior of the Al2O3 Doped Mesoporous Monometallic Cu Catalysts in Dimethyl Oxalate Hydrogenation Xiangpeng Kong1,2 · Yuehuan Wu1 · Peihong Yuan3 · Man Wang1 · Peng Wu2,4 · Lifeng Ding1 · Ruihong Wang1 · Jiangang Chen2 Received: 9 September 2020 / Accepted: 30 October 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract Al2O3 doped mesoporous monometallic Cu catalysts were successfully synthesized though the self-assembly Cu species derived from the oxalate precursor undergoing thermal decomposing. The evolutions of microstructures, physicochemical and surface properties of the CuAl catalysts have been systematically characterized focusing on the effect of the calcination temperature during catalyst preparation. It is found that the textural and surface properties of the CuAl catalysts were profoundly affected by the calcination temperature, further determining the resultant catalytic behavior in dimethyl oxalate (DMO) hydrogenation. Particularly, the CuAl-500 possessing the maximum surface C u+ sites and proper surface acid features exhibits 100.0% DMO conversion and 98.0% ethylene glycol (EG) selectivity in presence of the adequate active C u0 sites, which is superior to that of the other catalysts under the identical reaction conditions. And no activity loss occurred for more than 200 h demonstrated of the outstanding stability of the CuAl-500 catalyst. Moreover, the synergistic effect between surface C u+ and C u0 sites should be responsible for DMO selective hydrogenation. Additionally, the strengthened chemical interaction between Cu and Al species endows the catalysts outstanding stability by suppressing the dispersive Cu NPs agglomeration during DMO hydrogenation. Graphic Abstract
Keywords Mesoporous monometallic Cu catalysts · Al2O3 dopant · Dimethyl oxalate · Hydrogenation · Ethylene glycol * Xiangpeng Kong [email protected] * Jiangang Chen [email protected]; [email protected] 1
Department of Chemistry and Chemical Engineering, Taiyuan Institute of Technology, Taiyuan 030008, People’s Republic of China
2
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, People’s Republic of China
3
Taiyuan Institute of Mine Design and Research, Taiyuan 030012, People’s Republic of China
4
University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
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1 Introduction Ethylene glycol (EG), as a versatile fine chemicals and industrial intermediate, has been popular in the various chemical fields [1–3]. Currently, the feedstock for EG was mainly derived from the dwindling oil resource, hindering the desired production capacity [4–6]. Alternatively, syngas has been deemed as a promising stock for valuable chemical product, owing to the benign virtues of abundant resources, high atom economy and environmental benign [7–9]. Particularly, converting syngas to dimethyl oxalat
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