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  

Palladium catalyst supported on graphene oxide with temperaturesensitive surface and its catalytic performance

作　　者：丁雪洁 窦梦迪 李丹 鲁墨弘[1,2] 李明时 李永昕[1,2] 朱劼 DING Xuejie;DOU Mengdi;LI Dan;LU Mohong;LI Mingshi;LI Yongxin;ZHU Jie(Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou 213164,Jiangsu,China;School of Petrochemical Engineering,Changzhou University,Changzhou 213164,Jiangsu,China)

机构地区：[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

出　　处：《化工进展》2020年第5期1765-1773,共9页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(21676029,21761132006);江苏高校优势学科建设工程项目。

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。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/GOPNIPAM 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.

关 键 词：氧化石墨烯 聚(N-异丙基丙烯酰胺) 肉桂醛 加氢 

分 类 号：TQ612.3[化学工程—精细化工] O643.38[理学—物理化学]