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作 者:郭石菲 谢锐[1,2] 汪伟 巨晓洁[1,2] 刘壮 褚良银[1,2] GUO Shifei;XIE Rui;WANG Wei;JU Xiaojie;LIU Zhuang;CHU Liangyin(School of Chemical Engineering,Sichuan University,Chengdu 610065,Sichuan,China;State Key Laboratory of Polymer Materials Engineering,Sichuan University,Chengdu 610065,Sichuan,China)
机构地区:[1]四川大学化学工程学院,四川成都610065 [2]四川大学高分子材料工程国家重点实验室,四川成都610065
出 处:《化工进展》2020年第1期166-173,共8页Chemical Industry and Engineering Progress
基 金:国家自然科学基金(21622604);四川省杰出青年科技人才项目(2019JDJQ0026)
摘 要:利用聚多巴胺(PDA)的还原性和黏附性,成功制备了分别负载银(Ag)纳米催化剂的聚N-异丙基丙烯酰胺-聚多巴胺(PN@PDA/Ag)核壳型微球、聚苯乙烯-聚多巴胺(PS@PDA/Ag)核壳型微球和聚多巴胺(PDA/Ag)均质型微球。系统研究了PN@PDA/Ag、PS@PDA/Ag和PDA/Ag微球的微观结构、化学组成及Ag纳米颗粒的分布情况,并考察了在模型催化反应中,还原剂硼氢化钠(NaBH4)和反应物对硝基苯酚(4-NP)摩尔比对微球催化性能的影响。结果表明,3种微球均成功负载了Ag纳米催化剂,相比于两种核壳型微球,PDA/Ag微球负载Ag纳米催化剂的含量最多。随着NaBH4和4-NP摩尔比的增加,PN@PDA/Ag、PS@PDA/Ag和PDA/Ag微球对4-NP的转化率逐渐增大。在考察的摩尔比下,PDA/Ag微球均表现出比PN@PDA/Ag和PS@PDA/Ag微球更优异的催化性能。当摩尔比为500∶1时,PN@PDA/Ag、PS@PDA/Ag和PDA/Ag微球的表观反应速率常数(kapp)值分别为0.21min-1、0.35min-1和1.78min-1。PDA/Ag微球的kapp值远高于文献报道的PDA/Ag微球kapp的最大值0.35min-1。研究结果将为高效催化微球的设计和制备提供理论指导和实验基础。Threesilver(Ag)nanocatalystsloadedwithcore-shellpoly(N-isopropylacrylamide)-polydopamine(PN@PDA/Ag) microspheres, core-shell polystyrene-polydopamine(PS@PDA/Ag) microspheres andhomogeneous polydopamine(PDA/Ag) microspheres were successfully prepared by making use of thereducibility and adhesion of polydopamine(PDA). The microstructures, chemical compositions and thedistribution of Ag nanoparticles of PN@PDA/Ag, PS@PDA/Ag and PDA/Ag microspheres weresystematically studied. The effect of molar ratio of reductant sodium borohydride(NaBH4) to reactant p-nitrophenol(4-NP) on the catalytic performance of the three microspheres were investigated. The resultsshowed that Ag nanocatalysts were successfully loaded on all the three microspheres, and the amount of Agnanocatalysts loaded on PDA/Ag microspheres was the highest. With the increase of the molar ratio of NaBH4 to 4-NP, the conversions of 4-NP catalyzed by PN@PDA/Ag, PS@PDA/Ag and PDA/Ag microspheres all showed increasing trends. At all the molar ratios, PDA/Ag microspheres exhibited better catalyticperformance than the other two microspheres. When the molar ratio was 500∶1, the apparent kinetic rateconstants(kapp) of PN@PDA/Ag, PS@PDA/Ag and PDA/Ag microspheres were 0.21 min-1, 0.35 min-1 and1.78 min-1, respectively. The kapp of as-prepared PDA/Ag microspheres was much higher than the maximumone of 0.35 min-1 reported in literature. The results could provide theoretical guidance and experimental basis for the design and preparation of efficient catalytic polymeric microspheres.
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