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Carbon dioxide reduction in tandem with light-alkane dehydrogenation
Nature Reviews Chemistry ( IF 38.1 ) Pub Date : 2019-09-10 , DOI: 10.1038/s41570-019-0128-9
Elaine Gomez , Binhang Yan , Shyam Kattel , Jingguang G. Chen

A greenhouse gas and mild oxidant, CO2 can effect the oxidative dehydrogenation (CO2-ODH) of light alkanes over heterogeneous catalysts. These catalysts are bifunctional in that they mediate CO2 reduction while oxidizing the alkanes, most notably the C2–C4 components in shale gas. In this way, one obtains CO and alkenes as value-added products. Although desirable, this transformation has proven challenging in terms of catalyst design, with most catalysts for the CO2-ODH being metal oxides that typically undergo rapid deactivation. More recently, bimetallic catalysts have been identified as promising systems to activate alkanes by either selectively cleaving C–H bonds to produce alkenes or breaking all the C–C and C–H bonds to produce the dry reforming products CO and H2. This Review describes general trends in the CO2-ODH of light alkanes. We will also outline how to use a combined approach involving flow reactor experiments, in operando characterization and density functional theory to determine whether a catalyst is intrinsically active for CO2-ODH or dry reforming.



中文翻译:

轻烃脱氢串联减少二氧化碳

温室气体和温和的氧化剂CO 2可以在非均相催化剂上实现轻链烷烃的氧化脱氢(CO 2 -ODH)。这些催化剂是双功能的,因为它们在氧化烷烃的同时介导CO 2还原,最著名的是页岩气中的C 2 -C 4组分。以此方式,获得了CO和烯烃作为增值产品。尽管很理想,但事实证明这种转化在催化剂设计方面具有挑战性,其中大多数用于CO 2的催化剂-ODH是通常经历快速失活的金属氧化物。最近,双金属催化剂被认为是通过选择性裂解C–H键以生成烯烃或破坏所有C–C和C–H键以生成干重整产物CO和H 2来活化烷烃的有前途的系统。该评论描述了轻烷烃的CO 2 -ODH的一般趋势。我们还将概述在操作特性和密度泛函理论中如何使用涉及流动反应器实验的组合方法来确定催化剂对于CO 2 -ODH或干重整具有固有活性。

更新日期:2019-09-10
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