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全硅型分子筛组装GaN-ZnO固溶体催化CO2氧化丙烷脱氢制丙烯研究
结题报告
批准号:
22002143
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
宋健
依托单位:
学科分类:
催化化学
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
宋健
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中文摘要
当前,我国丙烯行业存在较大的供需缺口。以丰富且价廉的丙烷为原料进行CO2氧化脱氢获得高附加值的丙烯能够实现CO2资源化利用,缓解丙烯短缺问题,是一条更加经济合理的丙烯生产途径。然而,所报道的CO2氧化丙烷脱氢制丙烯催化剂大都活性不高,CO2对丙烷脱氢反应的促进作用不明显,且催化剂普遍失活较快,稳定性有待提高。本项目拟将弱酸性的镓物种与电子富集的氧化锌以GaN-ZnO固溶体的形式复合构筑催化剂,实现酸碱协同催化CO2氧化丙烷脱氢制丙烯反应;并进一步将GaN-ZnO固溶体组装在全硅型分子筛的孔道内实现活性位的高度分散,同时借助全硅型分子筛提供的特殊孔道结构赋予催化剂优异的性能;采用原位表征技术分析检测丙烷和CO2分子在催化剂表面的吸附、活化行为以及积炭物种的形成机制。在此基础上,优化全硅分子筛孔道内固溶体的电子结构和局部孔道环境,以获得高性能催化剂,为CO2氧化丙烷脱氢制丙烯工业应用奠定基础。
英文摘要
Currently, there is a huge gap between the supply and demand of propene in China. CO2 oxidative dehydrogenation of rich and low-cost propane can not only obtain high value-added propene to alleviate the shortage of propene, but also achieve the effective utilization of CO2, which is a more ideal choice for propene production. However, most of reported catalysts show poor activities, insufficient promotion role of CO2 and quick deactivation in CO2 oxidative dehydrogenation of propane to propene, and their stabilities need to be increased. Here, this project tends to construct a solid solution catalyst by combining weak acidity gallium species with electron-rich ZnO, thus resulting in an acid-base co-catalytic dehydrogenation of propane to propene with CO2. Furthermore, GaN-ZnO solid solution was confined in the channels of all-silicon zeolite to achieve much better dispersion of active sites, and the special structures of zeolite endows catalysts with excellent properties. The adsorption and activation mechanism of propane and CO2 and the deposition process of carbon species on the surfaces of catalysts are studied by in-situ characterizations. Based on these researches, efficient catalysts for CO2 oxidative dehydrogenation of propane to propene are expected to obtain to lay the foundation for its industrial application by optimizing the electronic properties and local porous environments of GaN-ZnO solid solution embedded in all-silicon zeolite.
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DOI:--
发表时间:2023
期刊:化学工业与工程
影响因子:--
作者:于芳;祖荣艳;吕云鹏;韩兴华;王志鹏;李裕;宋健
通讯作者:宋健
DOI:10.1007/s11595-023-2839-5
发表时间:2023-11
期刊:Journal of Wuhan University of Technology-Mater. Sci. Ed.
影响因子:--
作者:Bibo Li;Xiufang Dong;Yu Li;Jian Song;W. Xie;Wei Zhang;Yunfei Liu
通讯作者:Bibo Li;Xiufang Dong;Yu Li;Jian Song;W. Xie;Wei Zhang;Yunfei Liu
DOI:10.1016/j.micromeso.2023.112877
发表时间:2023-10
期刊:Microporous and Mesoporous Materials
影响因子:5.2
作者:Jian Song;Qing Miao;Yunpeng Lv;Zhipeng Wang;Yu Li;Liyan Wang;Mei Dong;Pengfei Wang;
通讯作者:Jian Song;Qing Miao;Yunpeng Lv;Zhipeng Wang;Yu Li;Liyan Wang;Mei Dong;Pengfei Wang;
DOI:10.3390/nano12223970
发表时间:2022-11-10
期刊:Nanomaterials (Basel, Switzerland)
影响因子:--
作者:
通讯作者:
DOI:--
发表时间:2023
期刊:NEW JOURNAL OF CHEMISTRY
影响因子:3.3
作者:Yunpeng Lv;Fang Yu;Zhipeng Wang;Haiwei Liu;Liyan Wang;Jian Song;Yu Li;Guiqiu Huang;Jian Cui
通讯作者:Jian Cui
国内基金
海外基金