Hydrogenation of Carbon Dioxide to Dimethyl Ether on CuO–ZnO/ZSM-5 Catalysts: Comparison of Powder and Electrospun Structures

Aidin Nejadsalim, Hamid Reza Godini (Corresponding author), Sanjay Ramesh Kumar, Fausto Gallucci, Delf Kober, Aleksander Gurlo, Oliver Görke (Corresponding author)

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Abstract

The promising direct dimethyl ether (DME) production through CO2 hydrogenation was systematically analyzed in this research by synthesizing, characterizing, and testing several catalytic structures. In doing so, various combinations of precipitation and impregnation of copper- and zinc-oxides (CuO–ZnO) over a ZSM-5 zeolite structure were applied to synthesize the hybrid catalysts capable of hydrogenating carbon dioxide to methanol and dehydrating it to DME. The resulting catalytic structures, including the co-precipitated, sequentially precipitated, and sequentially impregnated CuO–ZnO/ZSM-5 catalysts, were prepared in the form of particle and electrospun fibers with distinguished chemical and structural features. They were then characterized using XRD, BET, XPS, ICP, TGA, SEM, and FIB-SEM/EDS analyses. Their catalytic performances were also tested and analyzed in light of their observed characteristics. It was observed that it is crucial to establish relatively small-size and well-distributed zeolite crystals across a hybrid catalytic structure to secure a distinguished DME selectivity and yield. This approach, along with other observed behaviors and the involved phenomena like catalyst particles and fibers, clusters of catalyst particles, or the whole catalytic bed, were analyzed and explained. In particular, the desired characteristics of a CuO–ZnO/ZSM-5 hybrid catalyst, synthesized in a single-pot processing of the precursors of all involved catalytically active elements, were found to be promising in guiding the future efforts in tailoring an efficient catalyst for this system.

Original languageEnglish
Article number7255
Number of pages31
JournalMaterials
Volume16
Issue number23
DOIs
Publication statusPublished - Dec 2023

Funding

The PhD fellowship provided to Aidin Nejadsalim by the Berlin Graduate School of Natural Sciences and Engineering (BIG-NSE) as a part of cluster of excellence Unifying Systems in Catalysis (UniSysCat), founded by Deutsche Forschungsgemeinschaft, (DFG, German Research Foundation), is highly appreciated. Authors would like to thank Christina Eichenauer for BET measurement, Maria Unterweger, and Hüseyin Küçükkeçeci for their efforts to perform XPS measurements, Johannes Schmidt for assisting in analysis and deconvoluting of the XPS curves, Harald Link for making ICP-OES measurements, Alexander Büchner for assisting with laboratory experiments, and Sara Filipa Alves Santos for making SEM at Technische Universität Berlin. The authors also acknowledge Holger Kropf for making FIB-SEM characterization at Helmholtz-Zentrum Berlin (HZB). We are also grateful to Michael Geske, Martin Konrad, Franziska Thimm, and Frank Rosowski for conducting the catalytic activity test and providing the corresponding data at BASCAT-UniCat BASF JointLab. Authors acknowledge support by the German Research Foundation and the Open Access Publication Fund of TU Berlin. This research was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy—EXC 2008–390540038—UniSysCat.

FundersFunder number
Deutsche ForschungsgemeinschaftEXC 2008–390540038

    Keywords

    • characterization
    • CO hydrogenation
    • CuO–ZnO
    • dimethyl ether
    • electrospinning
    • hybrid catalyst
    • ZSM-5

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