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通过铜基纳米相自燃烧在介孔结构酸性载体中受限生长用于由一氧化碳生产二甲醚

Confined Growth by Self-Combustion of a Cu-Based Nanophase into Mesostructured Acid Supports for DME Production from CO.

作者信息

Secci Fausto, Mameli Valentina, Sanna Angotzi Marco, Atzori Luciano, Piroddi Lorenza, Pinna Nicola, Mureddu Mauro, Cannas Carla

机构信息

Department of Chemical and Geological Sciences, University of Cagliari, S.S. 554 bivio per Sestu, 09042, Monserrato, CA, Italy.

Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali (INSTM), Via Giuseppe Giusti 9, 50121, Firenze, FI, Italy.

出版信息

Chempluschem. 2025 May;90(5):e202400760. doi: 10.1002/cplu.202400760. Epub 2025 Feb 4.

Abstract

This work deals with the design of nanocomposite hydrogenation-dehydration bifunctional catalysts for the one-pot conversion of CO to dimethyl ether (DME), focusing on obtaining a high and homogeneous dispersion of a Cu-based CO hydrogenation phase into the pores of mesostructured supports. Particularly, three aluminosilicate mesostructured acid catalysts with catalytic activity towards methanol dehydration and featuring different porous structures (Al-MCM-41, Al-SBA-15, Al-SBA-16) were synthesized and used as supports to host a CuO/ZnO/ZrO (CZZ) CO hydrogenation catalyst for methanol synthesis. The use of a mesostructured support allows to maximize the exposed surface of the CO reduction function by nanostructuring it through its confinement within the mesochannels, thus obtaining nanocomposite bifunctional catalysts with an ultra-small hydrogenation nanophase. The nanocomposites were obtained using an impregnation strategy combined with a self-combustion reaction, allowing to incorporate the CO reduction phase inside the mesopores. In all cases, the characterization shows that the hydrogenation phase species are highly and homogeneously dispersed into the supports as either small nanoparticles or as a nanolayer. The as-obtained nanocomposites were tested for their catalytic activity and the results discussed taking into account the structural, textural, and acidic properties of the supports and nanocomposites.

摘要

这项工作涉及用于将CO一锅法转化为二甲醚(DME)的纳米复合加氢-脱水双功能催化剂的设计,重点是使铜基CO加氢相在介孔结构载体的孔中获得高度均匀的分散。具体而言,合成了三种对甲醇脱水具有催化活性且具有不同多孔结构的硅铝酸盐介孔结构酸催化剂(Al-MCM-41、Al-SBA-15、Al-SBA-16),并用作载体来负载用于甲醇合成的CuO/ZnO/ZrO(CZZ)CO加氢催化剂。使用介孔结构载体能够通过将CO还原功能限制在介孔通道内使其纳米结构化,从而最大化其暴露表面,进而获得具有超小加氢纳米相的纳米复合双功能催化剂。这些纳米复合材料是采用浸渍策略与自燃烧反应相结合的方法制备的,从而能够将CO还原相引入介孔内。在所有情况下,表征结果表明,加氢相物种以小纳米颗粒或纳米层的形式高度均匀地分散在载体中。对所制备的纳米复合材料的催化活性进行了测试,并结合载体和纳米复合材料的结构、织构及酸性性质对结果进行了讨论。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6dde/12105452/135ddbda4bf6/CPLU-90-e202400760-g003.jpg

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