Cu Nanoparticles Inlaid Mesoporous Al2O3 As a High-Performance Bifunctional Catalyst for Ethanol Synthesis via Dimethyl Oxalate Hydrogenation

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• 作者：Yifeng Zhu ; Xiao Kong ; Xianqing Li ; Guoqiang Ding ; Yulei Zhu ; Yong-Wang Li
• 刊名：ACS Catalysis
• 出版年：2014
• 出版时间：October 3, 2014
• 年：2014
• 卷：4
• 期：10
• 页码：3612-3620
• 全文大小：547K
• ISSN：2155-5435

文摘

Ethanol synthesis from syngas via dimethyl oxalate (DMO) hydrogenation is of crucial importance for environment- and energy-related applications. Herein, we designed the bifunctional Cu nanoparticle (NP) inlaid mesoporous Al₂O₃ catalyst and first applied it to ethanol synthesis with high efficiency. The catalyst was made based on the spatial restriction strategy by pinning the Cu NPs on mesoporous Al₂O₃ to conquer the sintering problem and facilitate the stability (>200 h at 270 掳C), which has potential values in high-temperature and exothermic reactions. The plentiful pores, highly exposed and properly assembled Cu-acid sites, furnished the catalyst with high ethanol yield (鈭?4.9%). A structure-sensitive behavior that the intrinsic activity increases with the decreasing NP size was discussed. It was attributed to the change in metal鈥揳cid interfacial sites, morphology, and electronic structure and balance of surface Cu⁰鈥揅u⁺ species. The mechanism for DMO hydrogenation to ethanol involving activation of C鈺怬, C鈥揙, and O鈥揌 bands was also proposed. As cleavage of these bonds is a versatile tool to utilize bioderived molecules (e.g., polyols), the bifunctional catalysts can also be applied to hydrogenolysis of C鈥揙 bonds or etherification of O鈥揌 groups to produce various chemicals.

Keywords:

ethanol synthesis; copper; mesoporous Al₂O₃; stability; metal-acid; structure鈭抋ctivity relationship