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用于合成气生产中镍沸石催化剂优化的响应面方法

Response Surface Methodology for Ni-Zeolite Catalyst Optimization in Syngas Production.

作者信息

Alanazi Yousef M, Al-Fatesh Ahmed S, Al-Mubaddel Fahad S, Ibrahim Ahmed A, Fakeeha Anis H, Abasaeed Ahmed E, Al-Garadi Najib Y A, Osman Ahmed I

机构信息

Chemical Engineering Department, College of Engineering, King Saud University, Riyadh 11421, Saudi Arabia.

School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast, BT9 5AG Northern Ireland, U.K.

出版信息

ACS Omega. 2024 Sep 25;9(40):41636-41650. doi: 10.1021/acsomega.4c05617. eCollection 2024 Oct 8.

Abstract

This work addresses the problem of converting waste methane, a significant greenhouse gas, using customized nickel-zeolite catalysts to produce profitable syngas. The investigation employs 5 wt % of Ni on various zeolite supports with Si/Al ratios ranging from 13 to 25. Comprehensive characterization methods, including temperature-programmed reduction, N adsorption-desorption, and X-ray diffraction, were used to identify critical structural characteristics that greatly impact the catalyst's performance. The study indicates that the reducibility and basicity of the catalyst, the type of zeolite support, and the kind of carbon deposits formed during the reaction at 800 °C all influence the efficiency of methane conversion to syngas. The best catalyst was found to be 5Ni-Z3, which at 800 °C produced high conversion rates of carbon dioxide (60%) and methane (50%). Lastly, the response surface methodology, in conjunction with numerical simulation, was used to determine the best operating settings for maximizing syngas production with the 5Ni-Z3 catalyst. Reaction temperature, space velocity, and the methane-to-carbon dioxide feed ratio were considered in this analysis. With a methane conversion rate exceeding 92%, a carbon dioxide conversion rate exceeding 90%, and a hydrogen-to-carbon monoxide ratio of 1.00, the catalyst produced experimental results very similar to the SRM predictions when the reaction was conducted at conditions close to the predicted values [temperature around 845 °C, space velocity around 22,000 mL/(h·gcat), and feed ratio close to 0.94]. The effectiveness of the identified operating conditions for the dry reforming process is validated by the near alignment of expected and experimental outcomes.

摘要

这项工作致力于解决利用定制的镍沸石催化剂将重要温室气体废甲烷转化为可盈利合成气的问题。该研究采用了5 wt%的镍负载在各种硅铝比为13至25的沸石载体上。使用了包括程序升温还原、氮气吸附-脱附以及X射线衍射在内的综合表征方法,以确定对催化剂性能有重大影响的关键结构特征。研究表明,催化剂的还原性和碱性、沸石载体的类型以及在800℃反应过程中形成的积碳种类,都会影响甲烷转化为合成气的效率。发现最佳催化剂是5Ni-Z3,它在800℃时能产生较高的二氧化碳转化率(60%)和甲烷转化率(50%)。最后,结合数值模拟使用响应面方法,来确定使用5Ni-Z3催化剂使合成气产量最大化的最佳操作条件。该分析考虑了反应温度、空速以及甲烷与二氧化碳的进料比。当在接近预测值的条件下进行反应时[温度约845℃,空速约22,000 mL/(h·gcat),进料比接近0.94],该催化剂产生的实验结果与SRM预测非常相似,甲烷转化率超过92%,二氧化碳转化率超过90%,氢碳比为1.00。预期结果与实验结果的接近一致验证了所确定的干重整过程操作条件的有效性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d4c/11465259/f28e8f33b08c/ao4c05617_0001.jpg

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