燃料化学学报（中英文）2025，Vol.53Issue(10)：1458-1469,中插1-中插12,24.DOI:10.1016/S1872-5813(25)60569-X
乙烷氨氧化反应:分子筛骨架铝分布调变Sn/H-ZSM-5的金属路易斯酸性及其催化性能
Regulation of the metal Lewis acidity and performance in ethane ammoxidation of the Sn/H-ZSM-5 catalysts through altering the zeolite framework aluminum distribution
摘要
Abstract
Three series of H-ZSM-5 zeolites(T,S,and G-series)with different Si/Al ratios were hydrothermally synthesized by using tetraethyl orthosilicate(T),silica sol(S),and fumed silica(G),respectively,as the silicon source,so as to modulate the distribution of aluminum in the zeolite framework.Subsequently,three series of Sn/H-ZSM-5 catalysts were prepared by loading Sn metal via the in situ atom grafting method and their catalytic performance in the ethane ammoxidation reaction was evaluated in a fixed-bed reactor.The results indicate that the T-series Sn/H-ZSM-5 catalysts exhibit much better performance in the ethane ammoxidation;in particular,the T-series Sn/H-ZSM-5 catalyst with a Si/Al ratio of 10 achieves an ethane conversion of 10％a with a selectivity of 70％-90％to acetonitrile(viz.,an acetonitrile yield of 7％-9％).The characterization results of Co-ZSM-5 UV-vis-DRS and the Sn/H-ZSM-5 infrared spectroscopy reveal that with the increase of the Si/Al ratio,the fraction of framework aluminum in the straight channels increases gradually,whereas the fraction of framework aluminum in the channel intersections decreases accordingly,accompanying by a decrease of the amount of Sn-Lewis acid sites,which suggests that the Sn-Lewis acid sites are principally located in the channel intersections of the H-ZSM-5 zeolites.The selectivity to acetonitrile is positively proportional to the amount of Sn-Lewis acid sites and a higher L/B ratio(e.g.,L/B＞1)is conducive to the formation of acetonitrile on the Sn/H-ZSM-5 catalyst,suggesting that the Sn-Lewis acid sites act as the catalytically active sites in the ethane ammoxidation to form acetonitrile.关键词
乙烷氨氧化/原位原子移植/金属路易斯酸/骨架铝分布Key words
ethane ammoxidation/in situ atom grafting/metal Lewis acids/framework-aluminum distribution分类
化学化工引用本文复制引用
乔石磊,梁庭钰,陈佳玲,史爱华,王波,夏中科,王森,金放,周晓霞..乙烷氨氧化反应:分子筛骨架铝分布调变Sn/H-ZSM-5的金属路易斯酸性及其催化性能[J].燃料化学学报（中英文）,2025,53(10):1458-1469,中插1-中插12,24.基金项目
The project was supported by National Natural Science Foundation of China(22002114,22102124,52272099),Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(GCP2023005,GCP2024010)and Science Foundation of Wuhan Institute of Technology(X24D086,23QD85).国家自然科学基金(22002114,22102124,52272099),绿色化工过程教育部重点实验室开放基金(GCP2023005,GCP2024010)和武汉工程大学科学基金(X24D086,23QD85)资助 （22002114,22102124,52272099）
