摘要
探讨了Al_(2)O_(3)载体孔结构对FeMo/Al_(2)O_(3)预加氢脱硫(HDS)催化剂活性和选择性的影响,采用浸渍法制备了一系列具有不同孔结构的FeMo/Al_(2)O_(3)催化剂,并通过微型固定床技术对其在模拟焦炉煤气中COS、CS_(2)、C_(4)H_(4)S和C_(2)H_(4)的HDS活性和选择性进行了系统评价,通过N_(2)吸附-脱附、红外碳硫、XRD、NH_(3)-TPD、H_(2)-TPR、XPS、Raman以及HRTEM等技术对催化剂进行了表征。研究结果表明,Al_(2)O_(3)载体孔结构对催化剂活性相MoS_(2)有显著影响,从而影响加氢脱硫活性和选择性,其中较大孔径的载体更有利于COS和CS_(2)的有效转化,而较小孔径的载体则更倾向于促进C_(4)H_(4)S和C_(2)H_(4)的转化;此外,具有较大孔径的催化剂不仅展现出更低的积炭倾向,还通过提高Mo物种的分散性,有效调控了MoS_(2)片晶的生长尺寸和层数,从而在COS和CS_(2)的加氢脱硫活性上显示了优异性能。研究结果为高效HDS催化剂的设计与开发开辟了新途径。
This investigation examines the influence of the Al_(2)O_(3)support pore structure on the activity and selectivity of FeMo/Al_(2)O_(3)pre-hydrodesulfurization(HDS)catalysts.A series of FeMo/Al_(2)O_(3)catalysts with different pore structures were synthesized by the impregnation method.The catalytic HDS performance was evaluated by using COS,CS_(2),C_(4)H_(4)S and C_(2)H_(4) as the probe molecules in a micro-fixed bed reactor.The physico-chemical properties ofγ-Al_(2)O_(3)supports and the corresponding FeMo catalysts were characterized by using methods such as N_(2)-physisorption,infrared carbon-sulfur analysis instrument,XRD,NH_(3)-TPD,H_(2)-TPR,XPS,Raman and HRTEM.The results of the research indicate that the Al_(2)O_(3)carrier hole structure has a significant effect on the catalyst activity of MoS_(2) phase,which affects the hydrogen desulfurization activity and selectivity.Among them,the carrier of the larger pore diameter is more conducive to the effective conversion of COS and CS_(2),while the carrier of the smaller pore diameter is more inclined to promote the conversion of C_(4)H_(4)S and C_(2)H_(4).Furthermore,catalysts with larger pore sizes not only showed reduced tendencies for carbon accumulation but also enhanced the dispersion of Mo species,effectively modulating the growth dimensions and layer counts of MoS_(2) crystallites.This led to exceptional HDS activity performance for COS and CS_(2),offering novel avenues for the engineering and development of highly effective HDS catalysts.
作者
王龙龙
秦志峰
班红艳
李乃珍
杜朕屹
于峰
翟志强
吴琼笑
WANG Longlong;QIN Zhifeng;BAN Hongyan;LI Naizhen;DU Zhenyi;YU Feng;ZHAI Zhiqiang;WU Qiongxiao(College of Chemical Engineering and Technology,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Shanxi Dongyi Coal Electric Aluminum Group Co.,Ltd.,Xiaoyi 032200,Shanxi,China;Dongguan Energy Investment Group Co.,Ltd.,Dongguan 523000,Guangdong,China)
出处
《化工学报》
EI
CSCD
北大核心
2024年第10期3623-3638,共16页
CIESC Journal
基金
2020年度东莞市能源投资集团有限公司攻关项目
2023年度山西省吕梁市校地合作重点研发专项(2023XDHZ08)
2023年度山西省中央引导地方科技发展资金项目(YDZJSX20231C006)。
