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An integrated process of CO2 capture and in situ hydrogenation to formate using a tunable ethoxyl-functionalized amidine and Rh/bisphosphine system

机译:使用可调的乙氧基官能化am和Rh /双膦系统进行CO2捕集和原位加氢形成甲酸的集成过程

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An integrated process of CO2 capture and in situ hydrogenation into formate was achieved in 95-99% yield using a tunable ethoxyl-functionalized amidine and Rh/bisphosphine system, being regarded as an alternative carbon capture and utilization approach to supply fuel-related products, to circumvent the energy penalty in carbon capture and storage. CO2 was captured by non-volatile amidine derivatives with simultaneous activation to form zwitterionic amidinium carbonate, and subsequent hydrogenation was facilitated by Rh/bisphosphine. The adsorption capacity and hydrogenation efficiency can be optimized by tuning the ethoxyl side chain. Particularly, the alkanolamidine bearing an intramolecular hydrogen donor derived from 1,8-diazabicyclo[5.4.0]-undec-7-ene (DBU) gave both a high CO2 uptake (molar ratio of 0.95 : 1) and excellent hydrogenation yield (99%). Furthermore, the silica-supported alkanolamidine was readily recovered and reused with the retention of good performance. This kind of carbon capture and utilization pathway could be a potential energy-saving option for industrial upgrading of CO2 from waste to fuel-related products in a carbon neutral manner.
机译:使用可调的乙氧基官能化am和Rh /双膦系统,完成了二氧化碳捕集和原位加氢成甲酸的集成过程,产率为95-99%,被认为是一种替代性的碳捕集和利用方法,用于提供与燃料相关的产品,规避碳捕获和存储中的能源损失。 CO 2被不挥发的idine衍生物捕获并同时活化形成两性离子碳酸am盐,随后的Rh /双膦促进了氢化反应。可以通过调节乙氧基侧链来优化吸附能力和氢化效率。特别地,带有衍生自1,8-二氮杂双环[5.4.0]-十一碳-7-烯(DBU)的分子内氢供体的链烷lam啶既具有高的CO 2吸收率(摩尔比为0.95:1),又具有优异的氢化产率(99)。 %)。此外,容易回收并负载有二氧化硅的链烷酰胺基并保持良好的性能。这种以碳中和的方式将碳捕集和利用的途径可能是潜在的节能选择,可以将工业中的二氧化碳从废物转化为与燃料相关的产品。

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