Zr-mordenite catalysts were prepared by post-treatment method and H-mordenite catalyst was synthesized by hydrothermal method for the dimethyl ether carbonylation reaction. XRD, N2 adsorption/desorption, ICP-OES, SEM, TEM, UV–Vis, XPS, Raman, CO-TPD, NH3-TPD, 27Al MAS NMR, FTIR and Py-IR were employed to characterize the catalysts. The results demonstrated that part of Zr atoms existed in a tetrahedral coordination state after incorporating into the mordenite framework. Zirconium Lewis acid sites with the ability to absorb CO molecules were formed during this process although the amount of Brønsted acid sites in 8-member ring channels decreased upon the incorporation of zirconium. During the concentration of zirconium nitrate solution increased from 0.02 to 0.08 mol/L, the Zr-mordenite catalyst through post-treatment with 0.04 mol/L zirconium nitrate solution exhibited the best catalytic performance at 473 K and 1 MPa. Dimethyl ether conversion and methyl acetate selectivity increased to 78% and 96% respectively compared with H-mordenite catalyst. Schematic of Zr incorporating MOR framework

中文翻译：

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Zr掺入对丝光沸石催化二甲醚羰基化的影响

采用后处理法制备Zr-丝光沸石催化剂，水热法合成H-丝光沸石催化剂，用于二甲醚羰基化反应。XRD、N2 吸附/解吸、ICP-OES、SEM、TEM、UV-Vis、XPS、拉曼、CO-TPD、NH3-TPD、27Al MAS NMR、FTIR 和 Py-IR 用于表征催化剂。结果表明，部分Zr原子掺入丝光沸石骨架后以四面体配位状态存在。在此过程中形成了具有吸收 CO 分子能力的锆路易斯酸位点，尽管在掺入锆后 8 元环通道中的布朗斯台德酸位点数量减少。在硝酸锆溶液的浓度从 0.02 增加到 0.08 mol/L 期间，Zr-丝光沸石催化剂通过用 0. 04 mol/L硝酸锆溶液在473 K和1 MPa下表现出最好的催化性能。与H-丝光沸石催化剂相比，二甲醚转化率和乙酸甲酯选择性分别提高到78%和96%。Zr结合MOR框架的示意图