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有序介孔氧化铝负载催化剂上戊二酸的强化加氢:制备策略的影响解析。

Enhanced Hydrogenation of Levulinic Acid over Ordered Mesoporous Alumina-Supported Catalysts: Elucidating the Effect of Fabrication Strategy.

机构信息

Department of Chemical Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, Republic of Korea.

出版信息

ChemSusChem. 2022 Mar 8;15(5):e202102662. doi: 10.1002/cssc.202102662. Epub 2022 Feb 2.

Abstract

In this work, three types of alumina-supported bimetallic Ni-Cu catalysts [Ni-Cu/commercial non-ordered mesoporous alumina (CMA), Ni-Cu/ordered MA (OMA), and Ni-Cu-OMA] were prepared via different fabrication strategies and investigated in the conversion of levulinic acid (LA) into γ-valerolactone and 2-methyltetrahydrofuran (2-MTHF). This study employed characterization techniques and reactions to reveal the effects of the fabrication strategy on the activities of the catalysts. It was observed that the catalysts constructed on OM supports (Ni-Cu/OMA and Ni-Cu-OMA) displayed superior catalytic performance compared to those constructed on CM supports (Ni-Cu/CMA). Specifically, Ni-Cu-OMA, which was fabricated via the one-pot evaporation-induced self-assembly strategy, exhibited the best catalytic performance, achieving a complete conversion of LA and a high selectivity of 73.0 % toward 2-MTHF in a solvent-free reaction environment. The promising activity of Ni-Cu-OMA was ascribed to the well-dispersed active sites within the framework of the support, the enhanced metal-support interaction, and the highly efficient exploitation of the synergistic effect between Ni and Cu. Detailed post-characterization techniques were also employed to highlight the outstanding stability of Ni-Cu-OMA.

摘要

在这项工作中,通过不同的制备策略制备了三种氧化铝负载的双金属 Ni-Cu 催化剂[Ni-Cu/商业无序介孔氧化铝(CMA)、Ni-Cu/有序 MA(OMA)和 Ni-Cu-OMA],并研究了它们在将乙酰丙酸(LA)转化为γ-戊内酯和 2-甲基四氢呋喃(2-MTHF)中的应用。本研究采用了表征技术和反应来揭示制备策略对催化剂活性的影响。结果表明,在 OM 载体上构建的催化剂(Ni-Cu/OMA 和 Ni-Cu-OMA)比在 CM 载体上构建的催化剂(Ni-Cu/CMA)具有更好的催化性能。具体来说,通过一锅蒸发诱导自组装策略制备的 Ni-Cu-OMA 表现出最佳的催化性能,在无溶剂反应环境中完全转化 LA,对 2-MTHF 的选择性高达 73.0%。Ni-Cu-OMA 的优异活性归因于载体骨架内活性位的良好分散、增强的金属-载体相互作用以及 Ni 和 Cu 之间协同效应的高效利用。还采用了详细的后表征技术来突出 Ni-Cu-OMA 的出色稳定性。

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