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通过鸟粪石模板法从废水中制备Pd/Mg₃(PO₄)₂及其作为硝基芳烃加氢化学选择性催化剂的应用

Fabrication of Pd/Mg P O via a Struvite-Template Way from Wastewater and Application as Chemoselective Catalyst in Hydrogenation of Nitroarenes.

作者信息

Zhang Peng, Xu Shaonan, Wang Yan, Zhang Wei, Li Wenqing, Wei Cundi, Zhang Peiping, Miao Shiding

机构信息

Key Laboratory of Automobile Materials of Ministry of Education, School of Materials Science and Engineering, Solid Waste Recycling Engineering Research Center of Jilin Province, Open Research Laboratory for Physicochemical Testing Methods of Functional Minerals, Ministry of Natural Resources, Jilin University, Changchun, 130022, P. R. China.

School of Materials Science & Engineering Electron Microscopy Center, Jilin University, Changchun, 130012, P. R. China.

出版信息

Chemistry. 2021 Jul 21;27(41):10666-10676. doi: 10.1002/chem.202100684. Epub 2021 Jun 17.

DOI:10.1002/chem.202100684
PMID:34009699
Abstract

A highly efficient heterogeneous catalyst Pd/Mg P O was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg P O fibers/rods. Mg P O fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg P O showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T=90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg P O supports. The favorable adsorption of withdrawing groups (-NO ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.

摘要

通过将钯纳米颗粒(PdNPs)与介孔Mg₃(PO₄)₂纤维/棒相结合,制备了一种高效的非均相催化剂Pd/Mg₃(PO₄)₂。以鸟粪石为模板制备了具有超高比表面积的Mg₃(PO₄)₂纤维,鸟粪石由含氮和磷污染物的废水合成。该策略为从富营养化污染水中开发先进催化剂提供了一条新途径。复合催化剂Pd/Mg₃(PO₄)₂在硝基芳烃选择性加氢制苯胺反应中表现出优异的性能。以硝基苯加氢为例,在T = 90℃、P = 2.0 MPa的条件下,苯胺的转化率和选择性几乎达到100%。发现其优异性能源于PdNPs,纳米纤维Mg₃(PO₄)₂载体提供的电子转移增强了PdNPs的性能。通过Pd与鸟粪石热解产生的氧空位之间的协同效应,实现了吸电子基团(-NO₂)的良好吸附。该催化剂在循环使用后仍保持稳定,催化性能几乎没有下降。

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