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Experimental data-driven reaction network identification and uncertainty quantification of CO2-assisted ethane dehydrogenation over Ga2O3/Al2O3
Chemical Engineering Science ( IF 4.7 ) Pub Date : 2021-02-19 , DOI: 10.1016/j.ces.2021.116534
Weiqi Chen , Maximilian Cohen , Kewei Yu , Hsuan-Lan Wang , Weiqing Zheng , Dionisios G. Vlachos

We study ethane dehydrogenation's kinetics over a Ga2O3/Al2O3 catalyst in the absence and presence of CO2 and H2O. We identify the reaction network through the hypothesis of overall-reactions and reaction stoichiometry using judicious experiments by co-feeding combinations of C2H6, CO2, H2, and H2O and regeneration studies. We introduce an uncertainty quantification methodology, leveraging Bayesian inference, to assess the rate parameters' statistical confidence and trace the uncertainty sources and develop a data-driven kinetics model. The chief overall reactions include ethane dehydrogenation and hydrogenolysis, the reverse water–gas shift (RWGS), coke formation, and coke gasification. H2O retards the ethane dehydrogenation rate and increases the apparent activation energy from 52.4 to 177.3 kJ/mol. Both CO2 and H2O improve catalyst stability via the same mechanism: coke gasification. Raman characterization of the spent catalyst reveals nanocrystal graphite coke whose amount is reduced by H2O. The reaction-network identification and uncertainty quantification apply to other complex reaction systems.



中文翻译:

Ga 2 O 3 / Al 2 O 3上CO 2辅助乙烷脱氢的实验数据驱动反应网络识别和不确定度定量

我们研究了在不存在和存在CO 2和H 2 O的情况下,在Ga 2 O 3 / Al 2 O 3催化剂上进行乙烷脱氢的动力学。 C 2 H 6,CO 2,H 2和H 2的混合进料O和再生研究。我们引入不确定性量化方法,利用贝叶斯推断,评估速率参数的统计置信度,并追踪不确定性来源,并开发数据驱动的动力学模型。主要的总体反应包括乙烷脱氢和氢解,水煤气逆反应(RWGS),焦炭形成和焦炭气化。H 2 O延迟了乙烷的脱氢速度,并将表观活化能从52.4增加到177.3 kJ / mol。CO 2和H 2 O都通过相同的机制(焦炭气化)提高了催化剂的稳定性。用过的催化剂的拉曼表征显示出纳米晶石墨焦炭,其量减少了H 2。O.反应网络识别和不确定性量化适用于其他复杂的反应系统。

更新日期:2021-03-09
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