化工进展 ›› 2020, Vol. 39 ›› Issue (5): 1765-1773.doi: 10.16085/j.issn.1000-6613.2019-0917

• 工业催化 • 上一篇    下一篇

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

丁雪洁1,2(), 窦梦迪1,2, 李丹1,2, 鲁墨弘1,2, 李明时1,2, 李永昕1,2, 朱劼1,2()   

  1. 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
  • 发布日期:2020-05-25
  • 通讯作者: 朱劼 E-mail:1499588689@qq.com;zhujie@cczu.edu.cn
  • 作者简介:丁雪洁(1989—),女,硕士研究生,研究方向为纳米材料与工业催化。E-mail:1499588689@qq.com
  • 基金资助:
    国家自然科学基金(21676029);江苏高校优势学科建设工程项目

Palladium catalyst supported on graphene oxide with temperature-sensitive surface and its catalytic performance

Xuejie DING1,2(), Mengdi DOU1,2, Dan LI1,2, Mohong LU1,2, Mingshi LI1,2, Yongxin LI1,2, Jie ZHU1,2()   

  1. 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
  • Published:2020-05-25
  • Contact: Jie ZHU E-mail:1499588689@qq.com;zhujie@cczu.edu.cn

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

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.

Key words: graphene oxide, poly(N-isopropylacrylamide), cinnamaldehyde, hydrogenation

中图分类号: 

  • TQ612.3