高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

PEG辅助合成高分散AgNPs/USY催化剂及其对4-硝基苯酚的高效催化还原

刘浩阳1，潘博2，刘治刚3，张志会1，高文秀1，杨颜如1，杨苗苗1
  

  1. 1.吉林化工大学化学与制药工程学院

    2.吉林石化公司有机合成厂 3.吉林化工大学石油化工学院

  • 收稿日期:2025-09-28 修回日期:2025-10-30 网络首发:2025-11-21 发布日期:2025-11-21
  • 通讯作者: 张志会 E-mail:zhangzh@jlict.edu.cn
  • 基金资助:
    吉林省科技发展计划项目（项目编号：YDZJ202301ZYTS319）和吉林省教育厅科研规划项目（编号：JJKH20240303KJ）资助

PEG-assisted synthesis of highly dispersed AgNPs/USY catalysts and their efficient catalytic reduction of 4-nitrophenol

LIU Haoyang1, PAN Bo2, LIU Zhigang3, ZHANG Zhihui1*, GAO Wenxiu1, YANG Yanru1, YANG Miaomiao1   

  1. 1. School of Chemistry and Pharmaceutical Engineering, Jilin University of Chemical Technology

    2. Organic Synthesis Plant, Jilin Petrochemical Company 3. School of Petrochemical Engineering, Jilin University of Chemical Technology

  • Received:2025-09-28 Revised:2025-10-30 Online First:2025-11-21 Published:2025-11-21
  • Contact: Zhi-Hui Zhang E-mail:zhangzh@jlict.edu.cn
  • Supported by:
    Supported by the Jilin Provincial Science and Technology Development Program (No.YDZJ202301ZYTS319) and the Jilin Provincial Department of Education Research Planning Project (No.JJKH20240303KJ)

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摘要： 在贵金属催化体系中，实现贵金属纳米颗粒的高度均匀分散，同时构建强金属-载体相互作用，是抑制活性组分迁移与流失、提升催化剂本征活性及稳定性的关键因素. 本文通过聚乙二醇（PEG）辅助水热合成法调控银纳米粒子（AgNPs）的分散与锚定状态，制备了AgNPs/USY，并将其应用于4-硝基苯酚（4-NP）的催化加氢反应中. 以USY分子筛为载体、PEG为还原与稳定剂，通过调整PEG分子量与银负载量，制备出一系列AgNPs/USY催化剂，并借助X射线衍射（XRD）、扫描电子显微镜（SEM）、X射线光电子能谱（XPS）和N?吸附-脱附（BET）等手段对其结构进行表征. 结果表明，利用PEG的空间位阻效应及其与分子筛表面官能团的协同作用，可实现AgNPs在USY介孔通道内的高度分散和有效锚定，显著抑制AgNPs的聚集和流失. 在常温常压条件下，PEG-400辅助合成的5% AgNPs/USY对高浓度4-NP（500 ppm）表现出优异的催化活性，8 min内转化率超过99.9%，表观速率常数高达0.817 min?1；在七次循环后仍保持90%以上活性，其稳定性显著优于AgNPs/HY体系. 表征分析进一步证实，孔道内限域的AgNPs具有更高的抗氧化与抗流失能力，XPS结果显示循环后AgNPs/USY中单质银保留量为AgNPs/HY的2.07倍.

关键词: 银纳米粒子, USY, 4-硝基苯酚, 催化还原

Abstract: In precious metal catalytic systems, achieving a high degree of uniform dispersion of precious metal nanoparticles while establishing strong metal-support interactions is crucial for inhibiting the migration and loss of active components, as well as enhancing the intrinsic activity and stability of the catalyst. This study utilizes a polyethylene glycol (PEG)-assisted hydrothermal synthesis method to control the dispersion and anchoring state of silver nanoparticles (AgNPs), resulting in the preparation of AgNPs/USY, which are then applied in the catalytic hydrogenation reaction of 4-nitrophenol (4-NP). Using USY zeolite as the support and PEG as the reducing and stabilizing agent, a series of AgNPs/USY catalysts were prepared by adjusting the molecular weight of PEG and the silver loading. Their structures were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption-desorption (BET). The results indicate that the steric hindrance effect of PEG and its synergistic interaction with the functional groups on the zeolite surface enable the high dispersion and effective anchoring of AgNPs within the mesoporous channels of USY, significantly suppressing the aggregation and loss of AgNPs. Under ambient temperature and pressure conditions, the 5% AgNPs/USY synthesized with the aid of PEG-400 exhibited excellent catalytic activity for high concentrations of 4-NP (500 ppm), achieving a conversion rate exceeding 99.9% within 8 minutes, with an apparent rate constant as high as 0.817 min?1. After seven cycles, it maintained over 90% activity, demonstrating significantly superior stability compared to the AgNPs/HY system. Characterization analysis further confirmed that the AgNPs confined within the pores exhibited higher resistance to oxidation and loss. XPS results indicated that the retention of elemental silver in AgNPs/USY was 2.07 times that of AgNPs/HY after cycling.

Key words: silver nanoparticles, USY, 4-Nitrophenol; Catalytic reduction

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