Article Link: https://www.nature.com/articles/s41563-021-01183-0
中文报道:
科学网:https://paper.sciencenet.cn/htmlpaper/2022/1/20221287583198769725.shtm
研之成理推送:https://mp.weixin.qq.com/s/kp-iJpzULEE39XnI7Hjlig
Our cooperative article “Tandem catalysis with double-shelled hollow spheres” has been published in Nature Materials (DOI: 10.1038/s41563-021-01183-0).
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.

This work was completed under the joint guidance of Professor Weckhuysen of Utrecht University and Professor Wang Ye of Xiamen University. The co-first authors are Dr. Xiao Jiadong of Utrecht University in the Netherlands (now working at SHINJU University in Japan) and Cheng Kang, associate professor of Xiamen University. The research work was supported by the Dutch NWO MCEC project (www.mcec-researchcenter. NL) and the National Natural Science Foundation of China (No. 91945301, 22121001 and 22072120).