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不同硅/铝比Beta分子筛中金属和酸平衡对苯甲醚加氢脱氧反应的影响

Influence of Metal and Acid Balance on Beta Zeolites With Different Si/Al Ratios on Anisole Hydrodeoxygenation

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【作者】 薛雨佳赵嘉欣张传浩范彬彬李文林

【Author】 XUE Yujia;ZHAO Jiaxin;ZHANG Chuanhao;FAN Binbin;LI Wenlin;College of Chemical Engineering and Technology, Taiyuan University of Technology;

【通讯作者】 李文林;

【机构】 太原理工大学化学工程与技术学院

【摘要】 分子筛负载贵金属双功能催化剂广泛应用于生物质加氢脱氧反应中,然而,金属-酸平衡对生物质转化的反应规律尚不明确。基于此,以Pt(NH44Cl2为金属前驱体,采用浸渍法制备负载型的Pt/HBeta双功能催化剂,利用X射线粉末衍射、扫描电子电镜、N2吸附-脱附、X射线光电子能谱、透射电子显微镜和氨气-程序升温脱附等表征手段对催化剂晶体结构、金属分布和载体酸性等物化性质进行表征。在调变硅/铝摩尔比(n(SiO2)/n(Al2O3))为30、65以及纯硅的HBeta分子筛的基础上,制备Pt负载质量分数分别为0.2%、0.6%及1.0%的催化剂,研究催化剂金属-酸平衡对苯甲醚加氢脱氧反应性能及反应路径的影响。结果表明,降低HBeta硅/铝摩尔比,有利于金属Pt物种的分散,而Pt/HBeta在苯甲醚加氢脱氧(HDO)反应中的催化性能和反应路径取决于金属Pt的负载量和HBeta酸中心的协同效应,尤其是HBeta的酸量。此外,在不同硅/铝摩尔比、不同Pt负载量的Pt/HBeta催化剂中,具有良好金属-酸平衡的1.0%Pt/HBeta-2表现出优异的催化性能。

【Abstract】 Zeolite-supported noble metal bifunctional catalysts are widely used in biomass hydrodeoxygenation reactions. However, the reaction mechanism of biomass conversion under the effect of metal-acid balance still remains unclear. Based on this, Pt(NH44Cl2 was used as a metal precursor to prepare the supported Pt/HBeta bifunctional catalyst by impregnation method. The physico-chemical properties the catalyst, such as crystalline structure, metal distribution, and acidic properties, were extensively characterized by means of X-ray powder diffraction, scanning electron microscopy, N2 adsorption-desorption, X-ray photoelectron spectroscopy, transmission electron microscopy and ammonia-temperature programmed desorption. Based on HBeta zeolites with Si/Al molar ratios of 30, 65, and pure silica, catalysts with the Pt loadings of 0.2%, 0.6%, and 1.0%(mass fraction) were prepared, so as to investigate the effect of metal-acid balance of the catalysts on the performance and reaction pathway of anisole hydrodeoxygenation. The results indicate that reducing the Si/Al molar ratio of HBeta favors the dispersion of Pt species. The catalytic performance and reaction pathway of Pt/HBeta in anisole hydrodeoxygenation reaction depend on the loading of Pt and synergistic effect of HBeta acidity, especially the acid amount of HBeta. Furthermore, among the Pt/HBeta catalysts with different Si/Al molar ratios and Pt loadings, 1.0%Pt/HBeta-2 with a well-balanced metal-acid ratio exhibits excellent catalytic performance.

【基金】 国家重点研发项目(2020YFB0606405);国家自然科学基金项目(21576177);石油化工分子转化与反应工程全国重点实验室开放课题(24-ZC0607-0099)资助
  • 【文献出处】 石油学报(石油加工) ,Acta Petrolei Sinica(Petroleum Processing Section) , 编辑部邮箱 ,2025年03期
  • 【分类号】TK6;O643.36
  • 【网络出版时间】2025-02-24 18:16:00
  • 【下载频次】204
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