石油化工
石油化工
석유화공
PETROCHEMICAL TECHNOLOGY
2015年
1期
29-35
,共7页
银催化剂%环氧乙烷%乙烯环氧化反应%宏观动力学模型
銀催化劑%環氧乙烷%乙烯環氧化反應%宏觀動力學模型
은최화제%배양을완%을희배양화반응%굉관동역학모형
silver catalyst%ethylene oxide%ethylene epoxidation%macrokinetic model
针对B型银催化剂，提出以表面反应为控制步骤、乙烯与一个活性中心位上非解离吸附氧发生环氧化反应和乙烯与相邻多个活性中心位上解离吸附氧发生深度氧化反应的乙烯环氧化反应机理；考虑到抑制剂1，2-二氯乙烷的竞争吸附作用，引入有效总活性位点覆盖率概念，构建包含1，2-二氯乙烷影响因子项的乙烯环氧化宏观动力学模型。采用无梯度反应器进行B型银催化剂上乙烯环氧化合成环氧乙烷的宏观动力学实验，以单纯形优化方法进行非线性参数估值，建立了与实验数据良好吻合的B型银催化剂上乙烯环氧化宏观动力学模型。
針對B型銀催化劑，提齣以錶麵反應為控製步驟、乙烯與一箇活性中心位上非解離吸附氧髮生環氧化反應和乙烯與相鄰多箇活性中心位上解離吸附氧髮生深度氧化反應的乙烯環氧化反應機理；攷慮到抑製劑1，2-二氯乙烷的競爭吸附作用，引入有效總活性位點覆蓋率概唸，構建包含1，2-二氯乙烷影響因子項的乙烯環氧化宏觀動力學模型。採用無梯度反應器進行B型銀催化劑上乙烯環氧化閤成環氧乙烷的宏觀動力學實驗，以單純形優化方法進行非線性參數估值，建立瞭與實驗數據良好吻閤的B型銀催化劑上乙烯環氧化宏觀動力學模型。
침대B형은최화제，제출이표면반응위공제보취、을희여일개활성중심위상비해리흡부양발생배양화반응화을희여상린다개활성중심위상해리흡부양발생심도양화반응적을희배양화반응궤리；고필도억제제1，2-이록을완적경쟁흡부작용，인입유효총활성위점복개솔개념，구건포함1，2-이록을완영향인자항적을희배양화굉관동역학모형。채용무제도반응기진행B형은최화제상을희배양화합성배양을완적굉관동역학실험，이단순형우화방법진행비선성삼수고치，건립료여실험수거량호문합적B형은최화제상을희배양화굉관동역학모형。
Possible reaction mechanism for the epoxidation of ethylene to ethylene oxide over the B-type silver catalyst was investigated,in which it was proposed that with the surface chemical reactions as rate-controlling step,the epoxidation reaction would occur between ethylene and non-dissociated adsorbed oxygen on an active site,and the deep oxidation would occur between ethylene and dissociated adsorbed oxygenon the adjacent active sites. Considering the strong competitive adsorption of 1,2-dichloroethane inhibitor,a concept for effective surface coverage was presented and the macro-kinetic model for the ethylene epoxidation over the B-type silver catalyst was established. Macro-kinetic experiments were carried out in a gradientless reactor. And the parameters of the macro-kinetic model were estimated by means of the simplex optimization method. Statistical test showed that the macro-kinetic model established for the B-type silver catalyst agreed well with the experimental results.
