化工学报 ›› 2020, Vol. 71 ›› Issue (6): 2889-2899.DOI: 10.11949/0438-1157.20200075

• 材料化学工程与纳米技术 • 上一篇    下一篇

铜基石墨烯复合催化剂的合成与表征

王永胜(),兰小林,邱天,张新平,吴莹莹,陈莉,徐伟祥,郭栋杰,段正康()   

  1. 湘潭大学化工学院,环境友好与资源高效利用化工新技术湖南省协同创新中心,湖南 湘潭 411105
  • 收稿日期:2020-01-17 修回日期:2020-03-30 出版日期:2020-06-05 发布日期:2020-06-05
  • 通讯作者: 段正康
  • 作者简介:王永胜(1995—),男,硕士研究生,871585227@qq.com
  • 基金资助:
    国家自然科学基金项目(21576229)

Synthesis and characterization of copper-based graphene composite catalyst

Yongsheng WANG(),Xiaolin LAN,Tian QIU,Xinping ZHANG,Yingying WU,Li CHEN,Weixiang XU,Dongjie GUO,Zhengkang DUAN()   

  1. College of Chemical Engineering, Hunan Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization, Xiangtan University, Xiangtan 411105, Hunan, China
  • Received:2020-01-17 Revised:2020-03-30 Online:2020-06-05 Published:2020-06-05
  • Contact: Zhengkang DUAN

摘要:

采用原位水热法制备了Cu/rGO催化剂并引入对苯二甲酸(TPA)对Cu基石墨烯复合材料进行改性研究,探究了不同溶剂、水热时间、沉淀pH对引入TPA的Cu/rGO催化剂材料微观结构特性的影响。通过XRD、FT-IR、XPS和SEM表征技术分析了催化剂的形貌结构及物化性质。考察了催化剂用于二乙醇胺脱氢的催化性能。在V(乙醇)V(水)=1∶1为溶剂,沉淀pH为13.0,160℃水热10 h,制备的催化剂性能最好,亚氨基二乙酸收率为86.55%,与没有添加TPA的Cu/rGO催化剂相比收率提高20%。TPA的加入,增强了GO片层间的相互作用,增加了GO片层间的有机官能团,稳定Cu2O并使其结晶度较好,增加催化剂活性位点,以提高反应速率。且粒径约为10 nm左右的Cu纳米粒子均匀分布在褶皱状片层结构的rGO表面,提高催化剂抗烧结性能。

关键词: 催化剂, 氧化, 制备, 烧结, 还原氧化石墨烯, 对苯二甲酸

Abstract:

A Cu/rGO catalyst was prepared by in-situ hydrothermal method and terephthalic acid (TPA) was introduced to modify the copper-based graphene composite material. The effects of different solvents, hydrothermal time and precipitation pH on microstructure characteristics of Cu/rGO catalyst material introduced by TPA were investigated. The effect of different molar ratios of copper and melamine on the catalyst was studied. Scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 physical adsorption and desorption test (BET) were used to investigate the morphology and structure of the catalyst. The catalytic performance of the catalyst for the dehydrogenation of diethanolamine was investigated. The results showed that with ethanol and water volume ratio of 1∶1 for the bases for solvent, the pH of the solution was 13.0, and reaction under 160℃ for 10 h, the preparation of the catalyst performance was the best, IDA yield was 86.55%. Compared with Cu/rGO catalyst without TPA, the yield of iminodiacetic acid increased by 20%. The addition of TPA and GO showed the best reduction effect, the interaction between TPA and GO were the strongest and stable Cu2O, make its crystallinity better, and increase the catalyst active site, to improve the reaction rate. GO has a folded lamellar structure. After reduction, the Cu nanoparticles with a particle size of about 10 nm are evenly distributed on the rGO surface of the corrugated sheet structure to improve the anti-sintering performance of the catalyst.

Key words: catalyst, oxidation, preparation, sintering, reduced graphene oxide, terephthalic acid

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