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炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响
引用本文:雷佳契,段学志,钱刚,周兴贵. 炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响[J]. 化工学报, 2017, 68(2): 679-686. DOI: 10.11949/j.issn.0438-1157.20161026
作者姓名:雷佳契  段学志  钱刚  周兴贵
作者单位:化学工程联合国家重点实验室, 华东理工大学化工学院, 上海 200237
基金项目:国家自然科学基金项目(21306046);化学工程联合国家重点实验室开放课题项目(SKL-ChE-15C03)。
摘    要:采用等量浸渍法制备了具有相似平均粒径的活性炭(AC)和碳纳米管(CNTs)负载的Pt催化剂,并比较研究了非碱性条件下两种催化剂催化甘油氧化反应的性能。结果表明,炭载体对Pt-C复合物催化甘油氧化反应的活性、选择性和稳定性有重要影响。相对于Pt/CNTs催化剂,Pt/AC催化剂中Pt 4f结合能较低,导致其表面氧的覆盖度相对较高,因而抑制了甘油的吸附,降低了甘油氧化反应的初始活性;Pt/AC催化剂会促进甘油醛进一步氧化成甘油酸以及C3产物的氧化断键;Pt/AC催化剂失活的主要原因是氧中毒和中间产物的吸附,而Pt/CNTs催化剂的失活主要是由于甘油酸的吸附堵塞Pt表面的活性位造成的。

关 键 词:甘油  氧化  Pt-C复合物  载体  失活  
收稿时间:2016-07-21
修稿时间:2016-12-16

Effects of carbon support on glycerol oxidation over Pt-C composite catalysts in base-free conditions
LEI Jiaqi,DUAN Xuezhi,QIAN Gang,ZHOU Xinggui. Effects of carbon support on glycerol oxidation over Pt-C composite catalysts in base-free conditions[J]. Journal of Chemical Industry and Engineering(China), 2017, 68(2): 679-686. DOI: 10.11949/j.issn.0438-1157.20161026
Authors:LEI Jiaqi  DUAN Xuezhi  QIAN Gang  ZHOU Xinggui
Affiliation:State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
Abstract:Activated carbon (AC) and carbon nanotubes (CNTs) supported Pt catalysts with similar particle sizes prepared by incipient wetness impregnation method were used for study of base-free oxidation of glycerol. The results showed that carbon support of Pt-C composite catalysts had significant impact on reactivity, selectivity, and steady state of glycerol oxidation. Compared to Pt/CNTs catalyst, Pt/AC catalyst had a lower binding energy of Pt 4f leading to a higher oxygen coverage on catalyst surface which reduced glycerol adsorption and initial activity of glycerol oxidation. Pt/AC catalyst further favored oxidation of glyceraldehyde to glyceric acid and C-C bond cleavage of C3 products. With regards to catalyst deactivation, oxygen poison and adsorption of intermediates were main factors to Pt/AC catalyst while blockage of Pt active sites by adsorption of glyceric acid was a significant contributor to Pt/CNTs catalyst.
Keywords:glycerol  oxidation  Pt-C composite  support  deactivation  
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