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目的:通过对混合丁烯氧化脱氢过程进行反应表征,对由Zn Fe_2O_4和Co_9Bi_1Fe_3Mo_(12)O_(51)组成的双床层催化剂体系中存在的协同机理进行解释;将异构化反应过程纳入反应体系,得出混合丁烯转化率和丁二烯收率上升的原因。创新点:1.提出基于丁烯异构体在床层之间浓度重分布和异构化效应抑制作用的协同作用机理;2.设计验证实验,从直观角度证实机理,并优化了催化剂的装填量和装填顺序。方法:1.通过单一丁烯和混合丁烯的氧化脱氢反应,对单一催化剂和双床层催化剂进行反应评估,得到相关反应数据;2.通过设计对比实验,从改变参加反应物质的直观角度对协同机理进行验证和解释;3.对参加反应的双层床催化剂中两种催化剂的装填量和装填顺序进行优化,为进一步研究组合型催化剂提供实验基础。结论:1.Zn Fe_2O_4对两种2-丁烯有更优的催化效果,而Co_9Bi_1Fe_3Mo_(12)O_(51)对1-丁烯有更优的催化效果,由两者组成的双层床催化体系对单一丁烯和混合丁烯的反应效果都有所提升,证明两种催化剂之间存在协同效应。2.双层床催化剂体系中,两种催化剂之间的协同作用机理是:催化剂不同活性导致丁烯异构体在床层之间的浓度发生重分布,同时由于多种异构体同时存在抑制了异构化反应。3.对双层床催化剂体系的装填顺序和装填量的优化结果表明,Zn Fe_2O_4装填在上层,Co_9Bi_1Fe_3Mo_(12)O_(51)装填在下层,且两者比例处于4:6到6:4之间时催化效果最佳。
OBJECTIVE: To explain the synergistic mechanism existing in the dual-bed catalyst system consisting of Zn Fe 2 O 4 and Co 9 Ti 3 Fe 3 Mo 12 O 51 (51) by the reaction characterization of the oxidative dehydrogenation of mixed butenes. The isomerization reaction process The reaction system gave the reason for the increase of mixed butene conversion and butadiene yield. Innovative points: 1. Proposed synergetic mechanism based on the concentration distribution of butylene isomers between the bed and the inhibition of isomerization effect; 2. Design verification experiments to confirm the mechanism from an intuitive point of view, and optimize the catalyst loading Quantity and loading order. Through the oxidative dehydrogenation reaction of single butene and mixed butene, the reaction of single catalyst and double bed catalyst was evaluated and the related reaction data were obtained.2. Through the design of comparative experiments, from the perspective of changing the participation of reactive substances To verify and explain the synergetic mechanism; (3) To optimize the filling amount and loading sequence of the two catalysts in the bilayer catalyst, which provide the experimental basis for further study of the combined catalyst. Conclusions: 1.Zn Fe 2 O 4 has better catalytic effect on the two kinds of 2-butene, while Co 9 Ti 3 Fe 3 MoO 12 O 51 has better catalytic effect on 1-butene, The effect of the system on the reaction of single butenes and mixed butenes was improved, demonstrating the synergistic effect between the two catalysts. In the bilayer catalyst system, the synergistic mechanism between the two catalysts is that the different activity of the catalyst leads to the redistribution of the concentration of the butylene isomers between the beds, and at the same time due to the simultaneous inhibition of multiple isomers Isomerization reaction. The results show that Zn_ (Fe_2O_4) is packed in the upper layer and Co_9Bi_1Fe_3Mo_ (12) O_ (51) is packed in the lower layer, and the ratio of the two is between 4: 6 and 6: 4 Between the best catalytic effect.