摘要
MIL-101(Cr)是最重要的金属有机框架(MOFs)材料之一, 稳定的框架结构和超高的比表面积使其在众多科学领域得到了广泛研究和应用. 但是MIL-101(Cr)的合成条件比较苛刻, 且稳定性较强, 因此, 有关于其分级结构的研究报道仍比较少. 本文提出了一种简单制备分级纳米孔结构MIL-101(Cr)的方法, 即以乙酸作为调节剂, 采用水热合成的方法, 一步得到具有微孔-介孔-大孔分级结构的MIL-101(Cr)材料. 实验结果表明, 该分级结构的MIL-101(Cr)与无分级结构的MIL-101(Cr)相比, 其大分子染料吸附能力和催化能力均有显著提高. 而且分级结构MIL-101(Cr)负载了磷钨酸催化剂之后, 表现出了与均相催化剂(纯磷钨酸)相当的催化能力. 进一 步研究发现, 使用其他短碳链的一元羧酸作为调节剂, 如丙酸、 丁酸等, 也可获得类似分级纳米结构MIL-101(Cr).
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Acknowledgements
This work was supported by the National Key R&D Program of China (2017YFC1103800), a joint National Natural Science Foundation of China-Deutsche Forschungsgemeinschaft (NSFC-DFG) project (NSFC 51861135313, DFG JA466/39-1), Program for Changjiang Scholars and Innovative Research Team in University (IRT_15R22), the National Natural Science Foundation of China (51802094, U1663225, U1662134, 21711530705 and 21706199), International Science & Technology Cooperation Program of China (2015DFE52870), Hubei Provincial Natural Science Foundation of China (2016CFA033) and Hunan Provincial Natural Science Foundation of China (2018JJ3122), the S&T Program of Hunan Province, China (2018RS3084), the Science Research Project of Hunan Provincial Department of Education (18B294) and the Fundamental Research Funds for the Central Universities (19lgzd16).
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Author contributions Zhao T and Li S carried out all the experiments; Xiao YX, Chang G, and Tian G took part in the characterization; Janiak C conceived the project and revised the paper; Yang XY conceived the project, provided the idea, designed and guided the experiments, and supported scientific and technological platform. All authors contributed to the general discussion.
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Tian Zhao completed his PhD under the supervision of Prof. Christoph Janiak at the University of Düsseldorf and then moved to Wuhan University of Technology as a postdoctoral research associate, working on metal-organic frameworks (MOFs) in the group of Prof. Xiao-Yu Yang. His research mainly focuses on the design, syntheses and applications of hierarchically porous materials.
Christoph Janiak is a full professor for bioinorganic chemistry and catalysis at the University of Düsseldorf, with research interests in the synthesis and properties of metal- and porous-organic frameworks (MOFs, COFs), metal nanoparticles, ionic liquids and catalysis. Until 2018 he was a visiting professor at Wuhan University of Technology in China.
Xiao-Yu Yang received his PhD from Jilin University (co-educated at FUNDP of Belgium). After a postdoctoral fellowship at the FUNDP, he worked as a “Chargé de Recherches” at the FNRS in Belgium. He is currently working as full professor at Wuhan University of Technology and visiting professor at Harvard University. His research is aimed at hierarchical assembly techniques, novel porous systems, and hierarchical structured materials for the applications in energy, environment, catalysis and bioengineering.
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Template-free synthesis to micro-meso-macroporous hierarchy in nanostructured MIL-101(Cr) with enhanced catalytic activity
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Zhao, T., Li, S., Xiao, YX. et al. Template-free synthesis to micro-meso-macroporous hierarchy in nanostructured MIL-101(Cr) with enhanced catalytic activity. Sci. China Mater. 64, 252–258 (2021). https://doi.org/10.1007/s40843-020-1435-3
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DOI: https://doi.org/10.1007/s40843-020-1435-3