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一种具有温敏表面的氧化石墨烯负载钯催化剂的制备及催化性能
引用本文:丁雪洁,窦梦迪,李丹,鲁墨弘,李明时,李永昕,朱劼.一种具有温敏表面的氧化石墨烯负载钯催化剂的制备及催化性能[J].化工进展,2020,39(5):1765-1773.
作者姓名:丁雪洁  窦梦迪  李丹  鲁墨弘  李明时  李永昕  朱劼
作者单位:1.江苏省绿色催化材料与技术重点实验室,江苏 常州 213164;2.常州大学石油化工学院,江苏 常州 213164
基金项目:江苏高校优势学科建设工程项目;国家自然科学基金
摘    要:以过硫酸铵(APS)为引发剂,N-异丙基丙烯酰胺(NIPAM)为单体,在氧化石墨烯(GO)表面生长温敏高分子聚(N-异丙基丙烯酰胺)(PNIPAM),获得复合载体GO-PNIPAM,并通过水相浸渍还原法制备具有温度敏感特性的Pd催化剂(Pd/GO-PNIPAM)。采用红外光谱、差示量热、热重、元素分析、透射电镜和电感耦合等离子原子发射光谱对复合载体GO-PNIPAM和Pd催化剂进行表征。结果表明,PNIPAM在GO上的接枝率约占60%。GO-PNIPAM显示出明显的温敏效应,其最低临界溶液温度约37℃。Pd/GO-PNIPAM上Pd纳米颗粒的平均粒径为(4.70±0.85)nm,远小于Pd/GO中Pd平均粒径(8.79±2.68)nm。因此,PNIPAM在GO上的接枝为金属纳米颗粒的沉积提供了大量的锚定位点,有助于金属纳米颗粒在其上的分散。Pd/GO-PNIPAM在高温下(80℃)肉桂醛(CAL)的选择性加氢反应中显示出优良的催化性能,初始转换频率(initial TOF)达192.3min-1,高于GO负载Pd催化剂(Pd/GO,103.5min-1)。Pd/GO-PNIPAM较高的Pd纳米颗粒分散性和高温下对CAL良好的吸附性能协同作用,导致其催化活性提高。

关 键 词:氧化石墨烯  聚(N-异丙基丙烯酰胺)  肉桂醛  加氢  

Palladium catalyst supported on graphene oxide with temperature-sensitive surface and its catalytic performance
DING Xuejie,DOU Mengdi,LI Dan,LU Mohong,LI Mingshi,LI Yongxin,ZHU Jie.Palladium catalyst supported on graphene oxide with temperature-sensitive surface and its catalytic performance[J].Chemical Industry and Engineering Progress,2020,39(5):1765-1773.
Authors:DING Xuejie  DOU Mengdi  LI Dan  LU Mohong  LI Mingshi  LI Yongxin  ZHU Jie
Affiliation:1.Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Changzhou 213164, Jiangsu, China
2.School of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, China
Abstract:Thermo-sensitive poly(N-isopropylacrylamide) (PNIPAM) was grown on graphene oxide (GO) with ammonium persulfate (APS) as the initiator to prepar the composite GO-PNIPAM, which was further employed to support Pd catalyst (Pd/GO-PNIPAM). The GO-PNIPAM and its supported Pd catalyst were characterized by FTIR, DSC, TG, OEA, TEM and ICP-AES. The results showed that 60% of the PNIPAM had grafted on GO. The GO-PNIPAM exhibited obvious thermoresponsive effect and its lower critical solution temperature (LCST) was about 37℃. The Pd particles deposited on the Pd/GO-PNIPAM had smaller size (4.70nm±0.85nm) than those on Pd/GO (8.79nm±2.68nm) because the graft of PNIPAM on GO provided a great number of anchoring sites for the dispersion of Pd nanoparticles. The Pd/GO-PNIPAM showed excellent catalytic activity in the selective hydrogenation of cinnamaldehyde (CAL) at high temperature (80℃) and the initial TOF was 192.3min-1, higher than that of Pd/GO (about 103.5min-1). The good Pd dispersion of Pd/GO-PNIPAM as well as its great adsorption ability to reactants at high temperature jointly resulted in an enhancement to the catalytic activity.
Keywords:graphene oxide  poly(N-isopropylacrylamide)  cinnamaldehyde  hydrogenation  
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