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First-Generation Organic Reaction Intermediates in Zeolite Chemistry and Catalysis
Chemical Reviews ( IF 51.4 ) Pub Date : 2022-08-10 , DOI: 10.1021/acs.chemrev.2c00076
Xuan Gong 1 , Mustafa Çağlayan 2 , Yiru Ye 1 , Kun Liu 1 , Jorge Gascon 2 , Abhishek Dutta Chowdhury 1
Affiliation  

Zeolite chemistry and catalysis are expected to play a decisive role in the next decade(s) to build a more decentralized renewable feedstock-dependent sustainable society owing to the increased scrutiny over carbon emissions. Therefore, the lack of fundamental and mechanistic understanding of these processes is a critical “technical bottleneck” that must be eliminated to maximize economic value and minimize waste. We have identified, considering this objective, that the chemistry related to the first-generation reaction intermediates (i.e., carbocations, radicals, carbenes, ketenes, and carbanions) in zeolite chemistry and catalysis is highly underdeveloped or undervalued compared to other catalysis streams (e.g., homogeneous catalysis). This limitation can often be attributed to the technological restrictions to detect such “short-lived and highly reactive” intermediates at the interface (gas–solid/solid–liquid); however, the recent rise of sophisticated spectroscopic/analytical techniques (including under in situ/operando conditions) and modern data analysis methods collectively compete to unravel the impact of these organic intermediates. This comprehensive review summarizes the state-of-the-art first-generation organic reaction intermediates in zeolite chemistry and catalysis and evaluates their existing challenges and future prospects, to contribute significantly to the “circular carbon economy” initiatives.

中文翻译:

沸石化学和催化中的第一代有机反应中间体

由于对碳排放的审查日益严格,预计沸石化学和催化将在未来十年中发挥决定性作用,以建立一个更加分散的可再生原料依赖型可持续社会。因此,缺乏对这些过程的基本和机械理解是一个关键的“技术瓶颈”,必须消除它才能最大限度地提高经济价值和减少浪费。考虑到这一目标,我们已经确定,与其他催化流(例如,均相催化)。这种限制通常可以归因于在界面(气-固/固-液)检测这种“短寿命和高反应性”中间体的技术限制;然而,最近出现的复杂光谱/分析技术(包括在原位/操作条件下)和现代数据分析方法共同竞争揭示这些有机中间体的影响。这篇综合综述总结了沸石化学和催化领域最先进的第一代有机反应中间体,并评估了它们现有的挑战和未来前景,为“循环碳经济”倡议做出重大贡献。最近出现的复杂光谱/分析技术(包括在原位/操作条件下)和现代数据分析方法共同竞争揭示这些有机中间体的影响。这篇综合综述总结了沸石化学和催化领域最先进的第一代有机反应中间体,并评估了它们现有的挑战和未来前景,为“循环碳经济”倡议做出重大贡献。最近出现的复杂光谱/分析技术(包括在原位/操作条件下)和现代数据分析方法共同竞争揭示这些有机中间体的影响。这篇综合综述总结了沸石化学和催化领域最先进的第一代有机反应中间体,并评估了它们现有的挑战和未来前景,为“循环碳经济”倡议做出重大贡献。
更新日期:2022-08-10
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