化工进展 ›› 2023, Vol. 42 ›› Issue (10): 5223-5231.DOI: 10.16085/j.issn.1000-6613.2022-2123

• 工业催化 • 上一篇    下一篇

Au-Pd/MnO2催化剂的制备及其苯甲醇氧化性能

郭晓宇(), 李冬晨, 赵炜, 杜朕屹, 李晓良()   

  1. 太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024
  • 收稿日期:2022-11-16 修回日期:2022-12-31 出版日期:2023-10-15 发布日期:2023-11-11
  • 通讯作者: 李晓良
  • 作者简介:郭晓宇(1996—),男,硕士研究生,研究方向为催化氧化。E-mail: guoxiaoyu0823@link.tyut.edu.cn
  • 基金资助:
    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)

Preparation of Au-Pd/MnO2 catalyst and its catalytic performance for benzyl alcohol oxidation

GUO Xiaoyu(), LI Dongchen, ZHAO Wei, DU Zhenyi, LI Xiaoliang()   

  1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2022-11-16 Revised:2022-12-31 Online:2023-10-15 Published:2023-11-11
  • Contact: LI Xiaoliang

摘要:

以硫酸锰、过硫酸铵和硫酸铵为原料,通过水热法制备了三种不同形态的MnO2(α型、β型和γ型),并利用溶胶-固载法负载了活性组分AuPd,然后将所制备的Au-Pd/MnO2用于无溶剂条件下的苯甲醇催化氧化。实验结果表明:载体MnO2的形态对催化剂的反应活性具有显著影响,苯甲醇在Au-Pd/γ-MnO2催化剂上反应的转化频率(TOF)值可以达到68283h-1,明显优于Au-Pd/β-MnO2(62299h-1)和Au-Pd/α-MnO2(35280h-1)。此外,循环稳定性实验表明Au-Pd/MnO2催化剂具有良好的反应稳定性。同时,利用X射线衍射、N2吸脱附曲线、透射电子显微镜、X射线光电子能谱等分析手段对所制备的催化剂进行结构表征,发现较小的AuPd纳米颗粒尺寸、载体上丰富的氧空位浓度和催化剂上Pd0活性物种的较高含量是Au-Pd/γ-MnO2催化剂取得高活性的关键。

关键词: 苯甲醇, 催化氧化, 二氧化锰, 无溶剂

Abstract:

α-MnO2, β-MnO2 and γ-MnO2 were prapered respectively with manganese sulfate, ammonium persulfate and ammonium sulfate as reactant by using hydrothermal method. Subsquently, Au-Pd nanoparticles were loaded on the MnO2 by sol-immobiliazation method. Then the prepared Au-Pd/MnO2 catalysts were used for the catalytic oxidation of benzyl alcohol under solvent-free condition. The experimental results indicated that the morphology of the MnO2 significantly affected on the catalytic performance. The TOF value on Au-Pd/γ-MnO2 reached 68283h-1, which was much higher than those of Au-Pd/β-MnO2 (62299h-1) and Au-Pd/α-MnO2 (35280h-1). Furthermore, the cycle stability experiment demonstrated that Au-Pd/MnO2 catalysts manifested a high durability. Meanwhile, XRD, N2-BET, TEM and XPS were conducted to characterize the prepared catalysts, the corresponding results revealed that the excellent performance of Au-Pd/γ-MnO2 was attributed to the smaller Au-Pd nanoparticle size, the higher number of oxygen vacancies in γ-MnO2 and the higher content of Pd0 active species.

Key words: benzyl alcohol, catalytic oxidation, manganese dioxide, solvent-free

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