Ambient conversion of CO2 to hydrocarbons by biogenic and synthetic [Fe4S4] clusters
Ambient conversion of CO2 to hydrocarbons by biogenic and synthetic [Fe4S4] clusters
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DOI：
10.1038/s41929-018-0079-4
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发表时间：
2018-06-01
期刊：
影响因子：
37.8
通讯作者：
Hu, Yilin
中科院分区：
文献类型：
--
作者：
Stiebritz, Martin T.;Hiller, Caleb J.;Hu, Yilin
固氮酶的铁蛋白含有一个具有氧化还原活性的[Fe4S4]簇，它在电子传递和底物还原中起着关键作用。在这里，我们表明，铁蛋白的醋酸甲烷八叠球菌可以减少二氧化碳和CO的碳氢化合物在环境条件下。此外，我们证明，这种反应性是固有的[Fe4S4]簇，显示的能力的合成[Fe4S4]化合物催化相同的环境反应的解决方案。理论计算表明，反应机制，涉及一个类似的中间体，产生烃类产品后，质子耦合的电子转移和伴随的水分子的去除。这些结果提供了一个框架的机制调查的FeS为基础的活化和还原的CO2和CO，同时促进潜在的发展FeS催化剂能够常温下转化为燃料产品的CO2和CO。
The Fe protein of nitrogenase contains a redox active [Fe4S4] cluster that plays a key role in electron transfer and substrate reduction. Here we show that the Fe protein of Methanosarcina acetivorans can reduce CO2 and CO to hydrocarbons under ambient conditions. Further, we demonstrate that this reactivity is inherent to [Fe4S4] clusters, showing the ability of a synthetic [Fe4S4] compound to catalyse the same ambient reaction in solutions. Theoretical calculations suggest a reaction mechanism involving an aldehyde-like intermediate that gives rise to hydrocarbon products upon proton-coupled electron transfer and concomitant removal of water molecules. These results provide a framework for mechanistic investigations of FeS-based activation and reduction of CO2 and CO while facilitating potential development of FeS catalysts capable of ambient conversion of CO2 and CO into fuel products.