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通过简便的氢键辅助聚合和固定化方法合成分级 Fe3O4@聚(4-乙烯基吡啶-co-二乙烯基苯)@Au 纳米结构及其催化应用。

Facile hydrogen-bond-assisted polymerization and immobilization method to synthesize hierarchical Fe3O4@poly(4-vinylpyridine-co-divinylbenzene)@Au nanostructures and their catalytic applications.

机构信息

School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, PR China.

出版信息

Chem Asian J. 2013 Jun;8(6):1160-7. doi: 10.1002/asia.201201186. Epub 2013 Apr 5.

Abstract

Hierarchical Fe3O4@poly(4-vinylpyridine-co-divinylbenzene)@Au (Fe3O4@P(4-VP-DVB)@Au) nanostructures were fabricated successfully by means of a facile two-step synthesis process. In this study, well-defined core-shell Fe3O4@P(4-VP-DVB) microspheres were first prepared with a simple polymerization method, in which 4-VP was easily polymerized on the surface of Fe3O4 nanoparticles by means of strong hydrogen-bond interactions between -COOH groups on poly(acrylic acid)-modified Fe3O4 nanoparticles and a 4-VP monomer. HAuCl4 was adsorbed on the chains of a P(4-VP) shell and then reduced to Au nanoparticles by NaBH4, which were embedded into the P(4-VP) shell of the composite microspheres to finally form the Fe3O4@P(4-VP-DVB)@Au nanostructures. The obtained Fe3O4@P(4-VP-DVB)@Au catalysts with different Au loadings were applied in the reduction of 4-nitrophenol (4-NP) and exhibited excellent catalytic activity (up to 3025 h(-1) of turnover frequency), facile magnetic separation (up to 31.9 emu g(-1) of specific saturation magnetization), and good durability (over 98 % of conversion of 4-NP after ten runs of recyclable catalysis and almost negligible leaching of Au).

摘要

采用简便的两步合成法成功制备了分级结构的 Fe3O4@聚(4-乙烯基吡啶-co-二乙烯基苯)@Au(Fe3O4@P(4-VP-DVB)@Au)纳米结构。在这项研究中,首先采用简单的聚合方法制备了具有良好定义的核壳结构的 Fe3O4@P(4-VP-DVB)微球,其中通过聚(丙烯酸)修饰的 Fe3O4 纳米粒子表面上的-COOH 基团与 4-VP 单体之间的强氢键相互作用,4-VP 很容易在 Fe3O4 纳米粒子表面聚合。HAuCl4 被吸附在 P(4-VP)壳的链上,然后用 NaBH4 还原为 Au 纳米粒子,这些 Au 纳米粒子被嵌入到复合微球的 P(4-VP)壳中,最终形成 Fe3O4@P(4-VP-DVB)@Au 纳米结构。所获得的不同 Au 负载量的 Fe3O4@P(4-VP-DVB)@Au 催化剂用于 4-硝基苯酚(4-NP)的还原,表现出优异的催化活性(高达 3025 h-1 的周转频率)、易于磁分离(高达 31.9 emu g-1 的比饱和磁化强度)和良好的耐久性(在 10 次可回收催化循环中,4-NP 的转化率超过 98%,Au 的浸出率可忽略不计)。

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