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PtxZn/MSN催化剂的合成及其丙烷脱氢性能研究

王文欣1, 单译欧1, 宋佳欣1, 范晓强1, 于学华1, 孔莲1, 肖霞1, 解则安1, 赵震1,2   

  1. 1. 沈阳师范大学 2. 中国石油大学(北京)
  • 收稿日期:2025-01-10 修回日期:2025-02-22 网络首发:2025-03-05 发布日期:2025-03-05
  • 通讯作者: 赵震 E-mail:zhenzhao@cup.edu.cn
  • 基金资助:
    国家自然科学基金(批准号:22172101); 辽宁省应用基础研究计划项目(批准号:2023JH2/101600059); 辽宁省“兴辽英才”青年拔尖 人才计划 (批准号:XLYC2203138); 辽宁省属本科高校基本科研业务费专项资金(批准号:LJ212410166046)和沈阳师范大学重大项目孵化工程 项目资助

Synthesis of the PtxZn/MSN catalysts and the study of their propane dehydrogenation properties

WANG Wenxin1, SHAN Yiou1, SONG Jiaxin1, FAN Xiaoqiang1, YU Xuehua1, KONG Lian1, XIAO Xia1, XIE Zean1, ZHAO Zhen1,2   

  1. 1. Shenyang Normal University 2. China University of Petroleum
  • Received:2025-01-10 Revised:2025-02-22 Online First:2025-03-05 Published:2025-03-05
  • Contact: Zhaozhen E-mail:zhenzhao@cup.edu.cn
  • Supported by:
    Supported by National Natural Science Foundation of China (No.22172101); Liaoning Province Applied Basic Research Program (No.2023JH2/101600059); Liaoning Xingliao Talented Youth Top Talent Program (No.XLYC2203138); The Fundamental Research Funds for the Liaoning Universities (No.LJ212410166046); Major Incubation Program of Shenyang Normal University

摘要: 摘要 随着社会对丙烯需求的增长, 发展高效丙烯生产技术无论对于科学研究和经济发展都至关重要. 铂基催化剂由于其具有较高的丙烷C?H键活化能力和丙烯选择性, 在丙烷脱氢(PDH) 反应中得到了广泛的研究.然而在丙烷脱氢反应过程中由于Pt的烧结及积碳导致催化剂快速失活. 高稳定性小尺寸Pt基催化剂的开发至关重要. 本文以具有限域作用的二氧化硅纳米粒子(MSN) 为载体, 利用过渡金属锌为助剂调控活性组分铂的电子性质及几何结构, 制备了系列不同锌含量的PtxZn/MSN催化剂. 进行了XRD、N2吸附-解吸、拉曼光谱、CO-DRIFT、SEM、TEM和XPS表征, 并测试了PDH性能. 当锌负载量为0.5 wt%时, Pt0.5Zn/MSN催化剂展示了最高的PDH性能, 其中, 丙烷初始转化率为47.9%, 丙烯选择性为97.0%, 6 h反应后, 丙烷转化率仍保持在45.8%, 选择性在97.0%, 丙烯生成速率为0.82 mol/min·gcat. 对PtxZn/MSN催化剂进行了多种表征分析, 结果表明锌的加入使Pt颗粒分割为更小的Pt物种, 提高了Pt的分散度, 从而减少了副反应的发生, 提高了催化剂的稳定性.

关键词: Pt基催化剂, 过渡金属锌助剂, 介孔二氧化硅纳米粒子, 丙烷脱氢, 丙烯 

Abstract: Abstract With the increasing demand for propylene in society, the development of efficient propylene production technology is crucial for both science and economy. Platinum based catalysts have been widely studied in propane dehydrogenation (PDH) reactions due to their high ability to activate propane C-H bonds and selectivity towards propylene. Herein, PtxZn/MSN catalysts with different zinc loadings were prepared by impregnation method using mesoporous silica nanoparticles (MSN) with confinement effect as support, transition metal zinc as a promoter to control the electronic property and geometric structure of platinum. XRD, N2 adsorption-desorption, Raman, CO-DRIFT, SEM, TEM and XPS characterizations were carried out and the PDH performance was tested. When the zinc loading was 0.5 wt%, PtxZn/MSN catalyst showed the highest PDH activity with the initial propane conversion and propylene selectivity of 47.9% and 97.0%, respectively. After 6 hours of reaction, the propane conversion and propylene selectivity of was 45.8% and 97.0% with the propylene production rate was 0.82 mol/min·gcat. The characterization results demonstrated that the addition of Zn divided Pt particles into smaller Pt species, improved Pt dispersion, reduced the occurrence of side reactions, and therefore enhanced the stability of the catalyst.

Key words: Pt-based catalysts, transition metal Zn promoter, mesoporous silica nanoparticles, propane dehydrogenation, propylene

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