无机材料学报 ›› 2022, Vol. 37 ›› Issue (4): 404-412.DOI: 10.15541/jim20210261

• 研究论文 • 上一篇    下一篇

硅钛杂化介孔球负载金纳米粒子及其催化性能调控

马慧1(), 陶疆辉1, 王艳妮1, 韩玉1, 王亚斌1,2(), 丁秀萍3()   

  1. 1.延安大学 化学与化工学院, 陕西省化学反应工程重点实验室, 延安 716000
    2.西北工业大学 化学与化工学院, 西安710129
    3.中国科学院 青海盐湖研究所, 中国科学院盐湖资源综合高效利用重点实验室, 西宁 810008
  • 收稿日期:2021-04-20 修回日期:2021-07-11 出版日期:2022-04-20 网络出版日期:2021-07-12
  • 通讯作者: 王亚斌, 副教授. E-mail: ybw_bingerbingo@126.com;
    丁秀萍, 副研究员. E-mail: dingxp@isl.ac.cn
  • 作者简介:马慧(1996-), 女, 硕士研究生. E-mail: mh08201@163.com
  • 基金资助:
    国家自然科学基金(52063029);陕西省自然科学基础研究计划资助项目(2019JQ-104);国家大学生创新创业训练计划项目(S202010719001)

Gold Nanoparticles Supported on Silica & Titania Hybrid Mesoporous Spheres and Their Catalytic Performance Regulation

MA Hui1(), TAO Jianghui1, WANG Yanni1, HAN Yu1, WANG Yabin1,2(), DING Xiuping3()   

  1. 1. Shaanxi Key Laboratory of Chemical Reaction Engineering, College of Chemistry and Chemical Engineering, Yan’an University, Yan’an 716000, China
    2. School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an 710129, China
    3. Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, China
  • Received:2021-04-20 Revised:2021-07-11 Published:2022-04-20 Online:2021-07-12
  • Contact: WANG Yabin, associate professor. E-mail: ybw_bingerbingo@126.com;
    DING Xiuping, associate professor. E-mail: dingxp@isl.ac.cn
  • About author:MA Hui (1996-), female, Master candidate. E-mail: mh08201@163.com
  • Supported by:
    National Natural Science Foundation of China(52063029);Natural Science Basic Research Plan in Shaanxi Province of China(2019JQ-104);National Training Program of Innovation and Entrepreneurship for Undergraduates(S202010719001)

摘要:

以能源开发(如光解水制氢)及环境保护(如有机物降解)应用为目标, 负载型贵金属催化剂在设计、制备及理论研究方面已取得了长足的发展。本工作以具有特异形貌及结构的树枝状二氧化硅纳米球载体为基础, 通过溶胶-凝胶法在其孔道引入二氧化钛纳米颗粒形成硅钛杂化结构。通过有机改性技术, 在树枝状硅钛杂化纳米球表面接枝氨基官能团。然后, 通过浸渍法和硼氢化钠还原手段, 在杂化纳米球孔道负载超细金纳米粒子。不同手段表征结果显示实验成功制备了树枝状硅钛杂化纳米球负载金纳米颗粒复合材料。在模拟太阳光下, 所得催化剂光解水产氢量及速率为69.08 μmol·g-1和13.82 μmol·g-1·h-1, 约为对比样催化剂(树枝状二氧化硅纳米球负载金纳米粒子)的7倍。在无光条件下, 其降解对硝基苯酚的表观动力学常数为6.540×10-3 s-1, 约为对比样的17倍(0.372×10-3 s-1)。由此可见, 设计合成的新型催化剂展现出优越的多功能催化活性。

关键词: 树枝状纳米球, 硅钛杂化结构, 金纳米粒子, 光解水制氢, 对硝基苯酚还原

Abstract:

In order to exploit energy sources (like photocatalytic water splitting for hydrogen production) and protect environment (like organics degradation), supported noble metal catalysts have made considerable progress in terms of design, fabrication, and theory. Herein, based on the specific morphology and structure of dendritic mesoporous silica nanospheres (DMSNs), TiO2 nanoparticles (NPs) were introduced into the channels via Sol-Gel method, developing dendritic mesoporous silica&titania nanospheres (DMSTNs). Then, amino groups (-NH2) were grafted onto DMSTNs surfaces by organic modification technology. Finally, ultrasmall gold (Au) NPs were anchored onto the as-prepared DMSTNs-NH2 through impregnation method and sodium borohydride (NaBH4) reduction. DMSTNs supported Au NPs catalysts could be successfully constructed, as verified by different methods. Under simulated sunlight for splitting water, the amount of produced H2 by the brand-new catalysts and the corresponding rate are 69.08 µmol·g-1 and 13.82 µmol·g-1·h-1, respectively, roughly. seven times of that of the contrast sample (DMSNs supported Au NPs). Without light irradiation, the apparent kinetic constant of p-nitrophenol reduction by the as-prepared catalysts is 6.540×10-3 s-1, about 17 times higher than that of the reference (0.372×10-3 s-1). ln conclusion, DMSTNs supported Au NPs exhibit good multifunctional catalytic activity.

Key words: dendritic nanospheres, silica&titania hybrid, gold nanoparticles, photocatalytic water splitting for hydrogen production, p-nitrophenol reduction

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