Abstract:

Carbonylation of dimethyl ether over mordenite has gained great attentions due to its mild reaction conditions and high product selectivity. The unique structure of mordenite endows it high catalytic efficiency, but mordenite also has the problems of carbon deactivation, short lifetime and poor stability. This paper summarizes the progress of mordenite modification in recent years towards overcoming the above problems. The modification methods are divided into four categories, namely acid sites regulation, mesopore introduction, morphology and grain size control and metal modification. These four methods can improve the activity and stability of mordenite catalyst by regulating the number of active sites, enhancing the mass transfer efficiency, or inhibiting coke deposition, respectively. Based on the existing results, the future modification of mordenite should be focused on removing the coking sites in the channels by methods for high-efficient mass transfer.

Key words: carbonylation, dimethyl ether, zeolite, modification, reaction, mass transfer

摘要：

丝光沸石催化二甲醚羰基化反应具有反应条件温和、产物选择性高等优点，近年来逐渐成为研究热点。丝光沸石因具有独特的结构，对二甲醚羰基化反应具有较高的催化效率，但同时也存在易积炭失活、寿命短、稳定性较差的问题。本文介绍了近年来研究人员为了克服上述问题对丝光沸石进行的各种改性研究的进展。目前，常用的改性方法包括酸中心调控、介微孔复合、形貌与晶粒尺寸调控和金属修饰四类，四种改性方法可通过调节反应活性中心数量、提高传质效率及抑制积炭来提高丝光沸石催化剂的活性和稳定性，但各有侧重。基于现有成果，丝光沸石催化剂下一步的改性研究重点是在强化传质的前提下通过各种方法来脱除或消灭位于传质通道中的积炭中心。

关键词: 羰基化, 二甲醚, 沸石, 改性, 反应, 传质