Sequential Hydrogenation of CO2 to Methanol Using a Pincer Iron Catalyst,Organometallics

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Sequential Hydrogenation of CO2 to Methanol Using a Pincer Iron Catalyst
Organometallics ( IF 2.5 ) Pub Date : 2019-07-29 , DOI: 10.1021/acs.organomet.9b00413
Elizabeth M. Lane ₁ , Yuanyuan Zhang ₂ , Nilay Hazari ₃ , Wesley H. Bernskoetter ₂

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Methanol is a crucial precursor for the preparation of many high-value commercial chemicals and synthesizing it from an inexpensive and renewable carbon source such as carbon dioxide (CO₂) could have significant benefits. Herein, a homogeneous iron(II) pincer complex for the catalytic generation of methanol from CO₂ and H₂ via a two-step process is described. The CO₂ reduction process occurs through initial coupling with H₂ and an amine to give a formamide. Subsequently, the formamide undergoes catalytic deaminative hydrogenation to afford methanol and regenerate the amine. A net turnover number of 590 is obtained for CO₂ and H₂ to methanol using this method. The primary obstacle to a single-batch catalytic process is CO₂ poisoning of the catalyst in the formamide hydrogenation step, and mechanistic investigations suggest that this CO₂ inhibition results from the formation of a stable iron(II) formate complex.

中文翻译：

使用cer铁催化剂将CO2连续加氢为甲醇

甲醇是制备许多高价值商业化学品的关键前体，由廉价且可再生的碳源（例如二氧化碳（CO ₂））合成甲醇具有巨大的优势。在此，描述了用于通过两步法从CO ₂和H ₂催化生成甲醇的均相铁（II）钳形络合物。CO ₂还原过程是通过与H ₂和胺的初始偶联而发生的，从而生成甲酰胺。随后，对甲酰胺进行催化脱氨基加氢以提供甲醇并再生胺。获得CO ₂和H _2的净营业额为590用这种方法将甲醇制得。单批催化过程的主要障碍是甲酰胺加氢步骤中催化剂的CO ₂中毒，并且机理研究表明，这种CO ₂抑制作用是由稳定的甲酸铁（II）配合物形成的。

更新日期：2019-07-30

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