SAPO-34催化剂上甲醇制烯烃反应——催化反应失活动力学  

Methanol to Olefins (MTO) Reaction over SAPO-34 Catalyst——Deactivation Kinetics of Catalytic Reaction

作　　者：齐国祯[1] 谢在库[2] 陈庆龄[1] 

机构地区：[1]中国石油化工股份有限公司上海石油化工研究院,上海201208 [2]中国石油化工股份有限公司,北京100728

出　　处：《化学反应工程与工艺》2013年第1期1-6,共6页Chemical Reaction Engineering and Technology

基　　金：国家重点基础研究发展规划(973计划)项目(2003CB615801);上海市科委重大基础研究项目(03DJ14004);中国石油化工股份有限公司重点科技攻关项目

摘　　要：甲醇制烯烃(MTO)催化剂SAPO-34在反应过程中存在失活现象,为了合理设计MTO反应器,需要了解该反应的本征动力学以及催化剂的失活规律,为此在固定床等温积分反应器内进行了甲醇制烯烃反应失活动力学的研究。通过测定不同催化反应时间下反应物和各产物的浓度,考察了催化剂不同使用时间后的催化活性,研究了SAPO-34催化剂的失活规律,建立了5集总反应和失活动力学模型,该模型充分考虑到水和积炭对反应过程的影响。根据实验测定的动力学数据拟合得到了失活反应的动力学常数,该动力学模型预测得到的SAPO-34催化剂上MTO反应产物组成随反应时间的变化规律与实验值吻合很好,说明了获得的动力学模型的可靠性。The SAPO-34 catalyst used for converting methanol to olefins （MTO） would be suffering deactivation by coking. In order to perform the rational design of MTO reactor, it is important to understand the intrinsic kinetics as well as the physics of catalyst deactivation. Experiments on MTO reaction in a fixed-bed isothermal integral reactor were carried out to study the deactivation of SAPO-34 catalyst. At different reaction time, the concentration of reactants and products were measured on stream, and catalytic activities were then determined. A kinetic model based on five-reaction deactivation mechanism was proposed, in which the influence of water and coke deposition was incorporated. The kinetic constants of deactivation reactions were obtained by regression of experimental data. A very good agreement between the model predictions and experimental data in terms of on-stream product concentration has been reached, which indicates that the kinetic model is reliable.

关 键 词：甲醇 烯烃 固定床反应器 积炭 失活动力学 

分 类 号：TQ013.2[化学工程]