TiO2氧空位含量对AuPd/TiO2催化氧化苯甲醇反应性能的影响
DOI:
CSTR:
作者:
作者单位:

1.太原理工大学;2.太原工业学院;3.福建理工大学

作者简介:

通讯作者:

中图分类号:

基金项目:

山西省基础研究计划(自由探索类)自然科学研究面上项目(20210302123093);来晋工作优秀博士(后)科研资助项目(2023LJ014);福建省自然科学基金(2023J01931),


The influence of TiO2 oxygen vacancy content on the catalytic performance of AuPd/TiO2 for benzyl alcohol oxidation
Author:
Affiliation:

1.Taiyuan University of Technology;2.Taiyuan Institute of Technology;3.Fujian University of Technology;4.Taiyuan University of Technology

Fund Project:

Free Exploration Project of Shanxi Basic Research Program(No. 20210302123093);Excellent Doctoral (Post-Doctoral) Scientific Research Funding Project for Working in Shanxi Province (2023LJ014);Natural Science Foundation of Fujian Province (No.2023J01931)

  • 摘要
  • |
  • 图/表
  • |
  • 访问统计
  • |
  • 参考文献
  • |
  • 相似文献
  • |
  • 引证文献
  • |
  • 资源附件
  • |
  • 文章评论
    摘要:

    以钛酸四丁酯为原料,采用水热法合成3种TiO2载体(TiO2-G、TiO2-E和TiO2-H),利用溶胶-固载法将活性组分Au、Pd负载在TiO2载体上制备了3种AuPd/TiO2,并将其应用于苯甲醇无溶剂催化氧化反应,结合XRD、XPS、N2-BET、EPR、TEM表征,考察TiO2载体不同氧空位含量对AuPd/TiO2催化苯甲醇无溶剂氧化反应性能的影响。结果表明,AuPd/TiO2-G具有最高的氧空位含量(0.198)、最小的AuPd纳米颗粒粒径(1.83 nm),其在120 ℃下催化氧化苯甲醇的反应中表现出最优异的催化性能,具有最高的TOF值(70554 h?1),明显优于AuPd/TiO2-H(39512 h-1)和AuPd/TiO2-E(14814 h-1);反应动力学实验结果表明,AuPd/TiO2-G具有最低反应表观活化能(55.77 kJ/mol),明显低于AuPd/TiO2-H( 72.78 kJ/mol)和AuPd/TiO2-E( 82.83 kJ/mol)。较高的载体氧空位含量有利于在催化剂表面形成较小尺寸的AuPd纳米颗粒和较高含量的表面Pd0物种,是AuPd/TiO2-G在苯甲醇氧化反应中取得优异催化活性的关键。

    Abstract:

    Three kinds of TiO2 supports (TiO2-G, TiO2-E and TiO2-H) were synthesized by using tetrabutyl titanate as raw material through hydrothermal method, and the active components Au and Pd were loaded onto the support by using sol-immobilization method to obtain three different AuPd/TiO2 catalysts, which were used for benzyl alcohol catalytic oxidation under solvent-free. By combining the characterizations of XRD, XPS, N2-BET, EPR and TEM, the influence of different oxygen vacancy contents in TiO2 carrier on the catalytic performance of AuPd/TiO2 in benzyl alcohol oxidation was investigated under solvent-free.The experimental results showed that the AuPd/TiO2-G with the highest oxygen vacancy content (0.198) and the smallest sized AuPd nanoparticles (1.83 nm) performed the best benzyl alcohol catalytic oxidation performance at 120 ℃, and the highest TOF value (70554 h-1) significantly better than AuPd/TiO2-H (39512 h-1) and AuPd/TiO2-E (14814 h-1 ). The reaction kinetics experiment results indicated that the AuPd/TiO2-G has the lowest apparent activation energy (55.77 kJ/mol), which is significantly lower than AuPd/TiO2-H (72.78 kJ/mol) and AuPd/TiO2-E (82.83 kJ/mol). A higher content of oxygen vacancy in the support is conducive to the formation of smaller-sized AuPd nanoparticles and a higher content of surface Pd0 species on the catalyst surface, which is the key to achieving the excellent catalytic activity of AuPd/TiO2-G in the benzyl alcohol catalytic oxidation reaction.

    参考文献
    相似文献
    引证文献
引用本文

李冬晨,郭晓宇,王哲,史荣会,赵炜,李晓良. TiO2氧空位含量对AuPd/TiO2催化氧化苯甲醇反应性能的影响[J].精细化工,2024,41(12):

复制
分享
文章指标
  • 点击次数:
  • 下载次数:
  • HTML阅读次数:
  • 引用次数:
历史
  • 收稿日期:2023-12-10
  • 最后修改日期:2024-04-07
  • 录用日期:2024-03-18
  • 在线发布日期: 2024-12-10
  • 出版日期:
文章二维码