Redox Oxide@Molten Salt as a generalized catalyst design strategy for oxidative dehydrogenation of ethane via selective hydrogen combustion
Redox Oxide@Molten Salt as a generalized catalyst design strategy for oxidative dehydrogenation of ethane via selective hydrogen combustion
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DOI：
10.1016/j.apcata.2022.118869
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发表时间：
2022-09
期刊：
影响因子：
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通讯作者：
Junchen Liu;S. Yusuf;Daniel Jackson;W. Martin;Dennis Chacko;Kyle Vogt-Lowell;Luke M. Neal;
中科院分区：
文献类型：
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作者：
Junchen Liu;S. Yusuf;Daniel Jackson;W. Martin;Dennis Chacko;Kyle Vogt-Lowell;Luke M. Neal;
目前的研究证明了氧化还原氧化物@熔盐核壳结构作为化学循环（乙烷氧化脱氢）的通用氧化还原催化剂设计策略。制备、评估和表征了 17 种氧化还原活性氧化物和熔盐的组合。 X射线衍射表明氧化还原氧化物和熔盐完全相容，形成独立且稳定的相。 X射线光电子能谱表明，熔盐聚集在氧化还原氧化物表面，形成核壳结构，以阻断负责COx形成的非选择性位点。使用所提出的氧化还原催化剂设计策略，单程烯烃收率高达~74%。性能数据的统计分析表明，通过使用本研究报告的氧化还原催化剂简单地优化操作条件，有可能实现高达 86.7% 的单程收率。同时，催化剂设计策略的通用性提供了令人兴奋的机会，可以在化学循环方案下进一步优化乙烷 ODH 氧化还原催化剂的组成和性能，并显着降低能耗和二氧化碳排放。
The current study demonstrates a redox oxide @ molten salt core-shell architecture as a generalized redox catalyst design strategy for chemical looping – oxidative dehydrogenation of ethane. 17 combinations of redox active oxides and molten salts were prepared, evaluated, and characterized. X-ray diffraction indicates that the redox oxides and molten salts are fully compatible, forming separate and stable phases. X-ray photoelectron spectroscopy demonstrates that the molten salts aggregate at the redox oxide surface, forming a core-shell structure to block the non-selective sites responsible for COxformation. Up to ∼74 % single-pass olefin yields were achieved using the proposed redox catalyst design strategy. Statistical analyses of the performance data indicate the potential to achieve up to 86.7 % single-pass yield by simply optimizing the operating conditions using the redox catalysts reported in this study. Meanwhile, the generalizability of the catalyst design strategy offers exciting opportunities to further optimize the composition and performance of the redox catalysts for ethane ODH under a chemical looping scheme with significantly reduced energy consumption and CO2emissions.