Mixed oxides as multi-functional reaction media for chemical looping catalysis
Mixed oxides as multi-functional reaction media for chemical looping catalysis
复制标题
混合氧化物作为化学链催化的多功能反应介质
DOI：
10.1039/d2cc05502c
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发表时间：
2022
影响因子：
4.9
通讯作者：
Li, Fanxing
中科院分区：
文献类型：
--
作者：
Liu, Junchen;Li, Fanxing
在过去的二十年中，化学链燃烧（CLC）已被广泛研究，作为一种有前途的方式来产生电力，同时产生浓缩的二氧化碳流用于封存。我们注意到，化学循环策略可以很好地扩展到基于燃烧的碳捕获之外。事实上，在燃烧以外的领域应用化学循环策略可以在根本不产生浓缩CO2流的情况下节省一些意想不到的能源和二氧化碳。此外，它允许基于循环的技术进入化学生产等应用-每年4万亿美元的高能源和碳强度工业部门。关键在于设计有效的氧载体，也称为通过化学链催化（CLCa）进行选择性化学转化的氧化还原催化剂。本文重点介绍了混合氧化物作为多功能反应介质在CLCa中的设计和应用。由于典型的混合氧化物氧载体往往是非选择性的烃类转化，本文的第一部分提出了一般的设计原则，表面改性的混合氧化物，以提高其选择性和催化活性。介绍了这些氧化还原催化剂在各种低碳烷烃和烷基苯化学链氧化脱氢反应中的应用。这是随后的讨论计算辅助混合氧化物设计的热力学标准的基础上。最后介绍了化学链技术的几个新发展方向。
Over the past two decades, chemical looping combustion (CLC) has been extensively investigated as a promising means to produce electric power while generating a concentrated carbon dioxide stream for sequestration. We note that the chemical looping strategy can be extended well outside of combustion-based carbon capture. In fact, application of the chemical looping strategy in areas beyond combustion can result in somewhat unexpected energy and carbon dioxide savings without producing a concentrated CO2 stream at all. Furthermore, it allows the looping-based technologies to tap into applications such as chemical production – a $4 trillion per year industrial sector with high energy and carbon intensities. The key resides in the design of effective oxygen carriers, also known as redox catalysts in the context of selective chemical conversion through chemical looping catalysis (CLCa). This contribution focuses on the design and applications of mixed oxides as multi-function reaction media in CLCa. Since typical mixed oxide oxygen carriers tend to be nonselective for hydrocarbon conversion, the first part of this article presents generalized design principles for surface modification of mixed oxides to improve their selectivity and catalytic activity. Applications of these redox catalysts in chemical looping – oxidative dehydrogenation (CL-ODH) of a variety of light alkanes and alkyl-benzenes are presented. This is followed with a discussion of computation assisted mixed oxide design based upon thermodynamic criteria. Finally, a few new directions for the chemical looping technologies are introduced.