首页|期刊导航|低碳化学与化工|Zn-Ag双金属改性丝光沸石催化剂在二甲醚羰基化反应中的性能研究

Zn-Ag双金属改性丝光沸石催化剂在二甲醚羰基化反应中的性能研究OA

Study on performance of Zn-Ag bimetallic modified mordenite catalyst in dimethyl ether carbonylation reaction

中文摘要英文摘要

针对二甲醚(DME)羰基化反应中丝光沸石(MOR)催化剂易失活问题,采用离子交换法引入Zn和Ag双金属对MOR进行改性,旨在优化其酸性位点分布及孔道结构以提升催化性能.通过水热合成法制备了系列催化剂,结合XRD、ICP-AES、SEM、NH3-TPD和Py-IR等表征手段分析了其物化性质,并在固定床反应器中评价了其催化活性.结果表明,引入Ag后,催化剂八元环孔道的Brønsted酸量和酸强度明显增大;引入Zn后,十二元环孔道的Lewis酸量增大,可协同促进CO吸附及反应动力学.在200℃、1.0 MPa及空速2400 mL/(g·h)条件下,1Ag/2Zn-MOR催化性能最优.在该催化剂作用下反应3 h时,DME转化率达98%;反应25 h后,DME转化率仍保持90%且乙酸甲酯选择性始终大于99%.Zn-Ag双金属改性通过调控催化剂酸位分布与孔结构,可有效提升催化活性与稳定性,为DME羰基化高效催化剂的开发提供了理论依据.

In response to the problem of easy deactivation of mordenite(MOR)catalyst in the dimethyl ether(DME)carbonylation reaction,the ion-exchange method was adopted to introduce Zn and Ag bimetals for the modification of MOR to optimize the distribution of acidic sites and the pore structure so as to enhance the catalytic performance.A series of catalysts were prepared by hydrothermal synthesis method,and their physicochemical properties were analyzed by characterization techniques,such as XRD,ICP-AES,SEM,NH3-TPD and Py-IR.The catalytic activity was evaluated in a fixed bed reactor.The results show that after the introduction of Ag,both the amount and strength of Brønsted acid in eight-membered ring channels of the catalyst increase significantly.After the introduction of Zn,the amount of Lewis acid in the twelve-membered ring channels increases,which synergistically promotes the adsorption of CO and the reaction kinetics.Under the conditions of 200℃,1.0 MPa and space velocity of 2400 mL/(g·h),the 1Ag/2Zn-MOR catalyst demonstrates the optimal catalytic performance.After reaction for 3 h with the catalyst,the conversion rate of DME reaches 98%.Even after reaction for 25 h,the DME conversion rate still remains 90%,and the selectivity of methyl acetate is always greater than 99%.The modification with Zn-Ag bimetals can effectively enhance the catalytic activity and stability by regulating the distribution of acid sites and the pore structure of the catalyst,which provides a theoretical foundation for the development of highly efficient catalysts for DME carbonylation.

余江峰;张海涛;马宏方;张皓荐;钱炜鑫;应卫勇

华东理工大学 化工学院 大型工业反应器工程教育部工程研究中心 化学工程联合国家重点实验室,上海 200237煤液化气化及高效低碳利用全国重点实验室,上海 200237华东理工大学 化工学院 大型工业反应器工程教育部工程研究中心 化学工程联合国家重点实验室,上海 200237煤液化气化及高效低碳利用全国重点实验室,上海 200237华东理工大学 化工学院 大型工业反应器工程教育部工程研究中心 化学工程联合国家重点实验室,上海 200237煤液化气化及高效低碳利用全国重点实验室,上海 200237

化学化工

二甲醚羰基化水热合成离子交换法丝光沸石双金属改性

dimethyl ether carbonylationhydrothermal synthesision-exchange methodmordenitebimetallic modification

《低碳化学与化工》 2026 (1)

54-62,9

国家自然科学基金(22178113)中央高校基本科研业务费专项资金(JKA01231712,JKCA1241202).

10.12434/j.issn.2097-2547.20250082

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