Fe3O4@P(St-co-OBEG)核壳结构微球负载银/铂纳米粒子复合催化剂的构筑及催化性能

doi:10.11896/cldb.201904001

材料导报

2019, Vol. 33

Issue (4): 571-576 https://doi.org/10.11896/cldb.201904001

无机非金属及其复合材料

Fe₃O₄@P(St-co-OBEG)核壳结构微球负载银/铂纳米粒子复合催化剂的构筑及催化性能

朱继红,曾碧榕,罗伟昂,袁丛辉,陈凌南,毛杰,戴李宗

厦门大学材料学院,福建省防火阻燃材料重点实验室,厦门 361005

Preparation and Catalytic Performance of Ag/Pt Nanoparticles Catalyst Supported on Fe₃O₄@P(St-co-OBEG) Core-Shell Structured Microspheres

ZHU Jihong, ZENG Birong, LUO Wei’ang, YUAN Conghui, CHEN Lingnan, MAO Jie, DAI Lizong

Fujian Key Laboratory of Fire Retardant Materials, College of Materials, Xiamen University, Xiamen 361005

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摘要本工作采用无皂乳液法合成出具有核壳结构的四氧化三铁@聚(苯乙烯-co-十八醇马来酸聚乙二醇双酯)(Fe₃O₄@P(St-co-OBEG))磁性聚合物复合微球,并以此为载体制备Ag/Fe₃O₄@P(St-co-OBEG)和Pt/Fe₃O₄@P(St-co-OBEG)两种复合催化剂。借助透射电镜和动态光散射表征复合催化剂的形貌和尺寸,并通过紫外可见吸光光度法测试它们的催化性能。实验结果表明两种复合催化剂对硝基苯和4-硝基苯酚的硝基加氢还原反应均具有良好的催化性能。相比Ag/Fe₃O₄@P(St-co-OBEG),Pt/Fe₃O₄@P(St-co-OBEG)催化活性更高,这可能与Pt/Fe₃O₄@P(St-co-OBEG)催化剂中Pt纳米粒子本身的高催化活性和在磁性聚合物载体上较大的比表面积有关,还有可能归因于Pt纳米粒子在Fe₃O₄@P(St-co-OBEG)上的分布更均匀。

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关键词: 四氧化三铁核壳结构聚合物载体磁性复合微球催化性能负载银铂纳米粒子

Abstract: In this work, magnetic composite microspheres Fe₃O₄@P(St-co-OBEG) were prepared via a surfactant-free emulsion polymerization and were used as carriers to support Ag and Pt to obtain magnetic composite nanocatalysts. It is known that magnetic composite catalysts can not only maintain the catalytic activity of noble metal nanoparticles, but realize magnetic separation. Here, the one-step surfactant-free emulsion polymerization was achieved by using styrene (St) as hydrophobic monomers, octadecyl-butenedioate-poly(ethylene glycol) (OBEG) as surfactant and γ-Fe₃O₄ as magnetic particles. Besides playing a role of surfactant to stable the solution, the amphiphilic oligomer OBEG also participated in the reaction during the polymerization. In details, the Fe₃O₄@P(St-co-OBEG) magnetic composite microspheres were prepared by stirring the reaction mixture at 65 ℃ for 24 h under N₂ atmosphere. TEM presented a clear core-shell structure of Fe₃O₄@P(St-co-OBEG) microspheres. The diameter of the core were about 100—120 nm, while the thickness of the shell was in the range of 30—50 nm. Moreover, particle size analysis based on dynamic light scattering (DLS) confirmed an average particle size of about 228 nm. Subsequently, Ag/Fe₃O₄@P(St-co-OBEG) and Pt/Fe₃O₄@P(St-co-OBEG) were prepared by simply reducing AgNO₃ or H₂PtCl₆ aqueous solution with dripping NaBH₄ under room tempe-rature, and the successful deposition of Ag or Pt nanoparticles on the surfaces of Fe₃O₄@P(St-co-OBEG) microspheres was observed. Through catalysis tests, both Ag/Fe₃O₄@P(St-co-OBEG) and Pt/Fe₃O₄@P(St-co-OBEG) can be regarded as efficient catalysts for the reduction reactions of hydrophobic nitrobenzene and hydrophilic 4-nitrophenol, in which Pt/Fe₃O₄@P(St-co-OBEG) performed better in catalytic activity compared with Ag/Fe₃O₄@P(St-co-OBEG). This might be attributed to the more uniform distribution of Pt nanoparticles than Ag nanoparticles on the surfaces of Fe₃O₄@P(St-co-OBEG) microspheres according to TEM observation.

Key words: ferroferric oxide core-shell structure polymer support magnetic composite microshperes catalytic property loading silver pla-tinum nanoparticles

出版日期: 2019-02-25 发布日期: 2019-03-11

ZTFLH:	O63
	TB3

基金资助: 国家自然科学基金(51573150;51673161);福建科技重大研发平台项目(2014H2006)

作者简介: 朱继红,厦门大学材料学院,2018年6月硕士研究生毕业。课题研究方向为纳米晶/双亲性聚合物杂化体的构筑,申报发明专利3项。戴李宗,博士,厦门大学特聘教授、博士研究生导师。福建省防火阻燃材料重点实验室主任,主要从事防火阻燃材料及功能高分子纳米复合材料的研究。在国内外重要期刊发表文章100多篇,获发明专利授权60余项。

引用本文:

朱继红, 曾碧榕, 罗伟昂, 袁丛辉, 陈凌南, 毛杰, 戴李宗. Fe₃O₄@P(St-co-OBEG)核壳结构微球负载银/铂纳米粒子复合催化剂的构筑及催化性能[J]. 材料导报, 2019, 33(4): 571-576.
ZHU Jihong, ZENG Birong, LUO Wei’ang, YUAN Conghui, CHEN Lingnan, MAO Jie, DAI Lizong. Preparation and Catalytic Performance of Ag/Pt Nanoparticles Catalyst Supported on Fe₃O₄@P(St-co-OBEG) Core-Shell Structured Microspheres. Materials Reports, 2019, 33(4): 571-576.

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http://www.mater-rep.com/CN/10.11896/cldb.201904001 或 http://www.mater-rep.com/CN/Y2019/V33/I4/571

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