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具有优异催化活性和可重复使用性的可磁回收还原氧化石墨烯纳米片/磁铁矿-钯气凝胶。

Magnetically recyclable reduced graphene oxide nanosheets/magnetite-palladium aerogel with superior catalytic activity and reusability.

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, China.

出版信息

J Colloid Interface Sci. 2017 Nov 15;506:154-161. doi: 10.1016/j.jcis.2017.07.036. Epub 2017 Jul 14.

Abstract

A two-step method was employed to synthesize reduced graphene oxide nanosheets/magnetite-palladium (rGSs/FeO-Pd) aerogel, with excellent catalytic activity and recyclability. Firstly, graphene oxide nanosheet (GS) hydrogels were formed by the self-assembly of GSs during the hydrothermal process. Meanwhile, hematite (α-FeO) and Pd nanoparticles (NPs) were synthesized and anchored onto the surface of the hydrogel. During heat-treatment, GSs were reduced to rGSs, while nonmagnetic α-FeONPs were converted to magnetic FeO NPs. The as-obtained rGSs/FeO-Pd aerogel displayed a three-dimensional interconnected hierarchical porous architecture, which was rich in mesopores and macropores. Such a structure was suitable for catalysis, since it not only improved the mass diffusion and transport, but also readily exposed the catalytic Pd NPs to the reactants. The typical reduction of 4-nitrophenol was chosen as a model reaction to evaluate the catalytic performance of the aerogel. As anticipated, both the reaction rate constant and turn over frequency of the aerogel were much higher than those of the commercial Pd/C catalyst. Moreover, due to incorporation of FeO NPs, the rGSs/FeO-Pd aerogel could be magnetically separated from the reaction solution and reused, without obvious loss of catalytic activity.

摘要

采用两步法合成了还原氧化石墨烯纳米片/磁铁矿-钯(rGSs/FeO-Pd)气凝胶,具有优异的催化活性和可回收性。首先,通过水热过程中 GSs 的自组装形成氧化石墨烯纳米片(GS)水凝胶。同时,合成并锚定了赤铁矿(α-FeO)和 Pd 纳米颗粒(NPs)到水凝胶的表面。在热处理过程中,GSs 被还原为 rGSs,而非磁性的α-FeONPs 被转化为磁性的 FeO NPs。所得到的 rGSs/FeO-Pd 气凝胶具有三维互连的分级多孔结构,富含中孔和大孔。这种结构有利于催化,因为它不仅提高了质量扩散和传输,而且还容易使催化 Pd NPs 暴露于反应物中。选择典型的 4-硝基苯酚还原作为模型反应来评估气凝胶的催化性能。正如预期的那样,气凝胶的反应速率常数和周转频率都远高于商业 Pd/C 催化剂。此外,由于 FeO NPs 的掺入,rGSs/FeO-Pd 气凝胶可以从反应溶液中通过磁性分离并重复使用,而催化活性没有明显损失。

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