Metal–zeolite composites with metal (oxide) and acid sites are promising catalysts for integrating multiple reactions in tandem to produce a wide variety of wanted products without separating or purifying the intermediates. However, the conventional design of such materials often leads to uncontrolled and non-ideal spatial distributions of the metal inside/on the zeolites, limiting their catalytic performance. Here we demonstrate a simple strategy for synthesizing double-shelled, contiguous metal oxide@zeolite hollow spheres (denoted as MO@ZEO DSHSs) with controllable structural parameters and chemical compositions. This involves the self-assembly of zeolite nanocrystals onto the surface of metal ion-containing carbon spheres followed by calcination and zeolite growth steps. The step-by-step formation mechanism of the material is revealed using mainly in situ Raman spectroscopy and X-ray diffraction and ex situ electron microscopy. We demonstrate that it is due to this structure that an Fe2O3@H-ZSM-5 DSHSs-showcase catalyst exhibits superior performance compared with various conventionally structured Fe2O3-H-ZSM-5 catalysts in gasoline production by the Fischer–Tropsch synthesis. This work is expected to advance the rational synthesis and research of hierarchically hollow, core–shell, multifunctional catalyst materials.
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Imaging Cu2O nanocube hollowing in solution by quantitative in situ X-ray ptychography
Nature Communications Open Access 29 August 2022
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B.M.W. acknowledges financial support from the Netherlands Organization for Scientific Research (NWO) in the frame of a Gravitation Program MCEC (Netherlands Center for Multiscale Catalytic Energy Conversion, www.mcec-researchcenter.nl). X.X. (Utrecht University) acknowledges financial support from the EU H2020-MSCA-ITN-2015 project ‘MULTIMAT’ (project no. 676045). K.C. and Y.W. acknowledge financial support from the National Natural Science Foundation of China (grant nos. 91945301, 22121001 and 22072120). J.X. thanks D. Wezendonk (Utrecht University) for his help with the in situ XRD measurements.
The authors declare no competing interests.
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Xiao, J., Cheng, K., Xie, X. et al. Tandem catalysis with double-shelled hollow spheres. Nat. Mater. 21, 572–579 (2022). https://doi.org/10.1038/s41563-021-01183-0
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