Methanol production from CO2via an integrated, formamide-assisted approach,Sustainable Energy & Fuels

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Methanol production from CO2via an integrated, formamide-assisted approach
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2020/01/07 , DOI: 10.1039/c9se01141b
Jorge G. Uranga _{1,

2,

3,

4,

5} , Aswin Gopakumar _{1,

2,

3,

4} , Tim Pfister _{1,

2,

3,

4} , Gunay Imanzade _{1,

2,

3,

4} , Loris Lombardo _{1,

1,

2,

3,

4} , Gabriela Gastelu _{5,

6,

7,

8,

9} , Andreas Züttel _{1,

2,

4,

10,

11} , Paul J. Dyson _{1,

2,

3,

4}

Affiliation

The synthesis of fuels from CO₂ has made tremendous progress in recent years, although practical applications remain limited. Herein, we describe a cyclic process that produces MeOH from CO₂via formamide intermediates, which are initially reduced using NaBH₄ to form methanol and concomitantly release the corresponding amine, from which the formamide is subsequently regenerated in the presence of CO₂/NaBH₄. By tuning the substituents on the formamide/amine, the selectivity of both steps can be controlled, allowing the process to proceed in high yields, either in two separate steps or in a single step process. The observed trends in reactivity were rationalized with a resonance model of the formamide, which supports the observed trends in reactivity, and further consolidated by spectroscopy and calculations.

中文翻译：

通过集成的甲酰胺辅助方法从二氧化碳中生产甲醇

尽管实际应用仍然有限，但近年来由CO ₂合成燃料已取得了巨大进展。本文中，我们描述了一种循环过程，该过程通过甲酰胺中间体从CO ₂中生产出MeOH ，该中间体最初使用NaBH ₄还原以形成甲醇，并同时释放出相应的胺，随后在CO ₂ / NaBH ₄存在下从中再生出甲酰胺。。通过调节甲酰胺/胺上的取代基，可以控制两个步骤的选择性，从而使该过程以高产率进行，可以分两个步骤进行，也可以分步进行。使用甲酰胺的共振模型合理化了观察到的反应性趋势，该模型支持了观察到的反应性趋势，并通过光谱和计算进一步合并。

更新日期：2020-03-31

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