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限域于介孔碳中的超细NiMoO纳米颗粒用于还原硝基芳烃：活性位点组成和可及性的影响

Ultrafine NiMoO nanoparticles confined in mesoporous carbon for the reduction of nitroarenes: effect of the composition and accessibility of the active sites.

作者信息

Li Shuna, Lv Yipin, Song Guolong, Li Cuncheng, Gao Daowei, Chen Guozhu

机构信息

School of Chemistry and Chemical Engineering, University of Jinan Jinan 250022 PR China

出版信息

RSC Adv. 2019 Feb 6;9(8):4571-4582. doi: 10.1039/c8ra09026b. eCollection 2019 Jan 30.

DOI:10.1039/c8ra09026b
PMID:35520158
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9060605/
Abstract

The design of ultrafine NiMoO nanoparticles (NPs) confined in hierarchically porous carbon remains a great challenge due to its high calcination temperature. In addition, the composition of active sites of NiMoO NPs for the hydrogenation reaction is still ambiguous. Herein, we report a general approach for the synthesis of ultrafine NiMoO NPs confined in mesoporous carbon with different morphologies and compositions using the replication method with SBA-15 as a hard template. The pore structure of mesoporous carbon and the Ni/Mo composition valence-state were discovered to be the main factors in the reduction of nitroarenes. The NiMoO /mesoporous carbon-platelet (NiMoO /MC-PL) with short mesochannels (∼350 nm) and high surface area (∼995 m g) possessed excellent catalytic activity towards the reduction of 4-nitrophenol, whereas NiMoO /mesoporous carbon-hexagonal-prism (NiMoO /MC-HP), NiMoO /mesoporous carbon-long-rod (NiMoO /MC-LR), and NiMoO /mesoporous carbon-spherical (NiMoO /MC-SP) with long mesochannels and relatively less surface area exhibited poor catalytic performance. The bifunctional mechanism or electronic synergistic effects of Ni and Mo species enhanced their catalytic performance. A good balance between MoO and metallic Ni (NiMoO /MC-PL-450) was found to be suitable for the reduction of 4-NP.

摘要

由于煅烧温度高，将超细NiMoO纳米颗粒（NPs）限制在分级多孔碳中进行设计仍然是一个巨大的挑战。此外，用于氢化反应的NiMoO NPs活性位点的组成仍不明确。在此，我们报道了一种通用方法，以SBA-15为硬模板，通过复制法合成了具有不同形态和组成的、限制在介孔碳中的超细NiMoO NPs。发现介孔碳的孔结构和Ni/Mo组成价态是还原硝基芳烃的主要因素。具有短介孔通道（约350 nm）和高表面积（约995 m²/g）的NiMoO/介孔碳片（NiMoO/MC-PL）对4-硝基苯酚的还原具有优异的催化活性，而具有长介孔通道和相对较小表面积的NiMoO/介孔碳六棱柱（NiMoO/MC-HP）、NiMoO/介孔碳长棒（NiMoO/MC-LR）和NiMoO/介孔碳球（NiMoO/MC-SP）表现出较差的催化性能。Ni和Mo物种的双功能机制或电子协同效应增强了它们的催化性能。发现MoO₃和金属Ni（NiMoO/MC-PL-450）之间的良好平衡适用于4-NP的还原。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/02f0/9060605/ec6318a29bc1/c8ra09026b-s2.jpg
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