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Widening the Product Profile of Carbon Dioxide Reduction by Vanadium Nitrogenase
Author(s) -
Rebelein Johannes G.,
Hu Yilin,
Ribbe Markus W.
Publication year - 2015
Publication title -
chembiochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.05
H-Index - 126
eISSN - 1439-7633
pISSN - 1439-4227
DOI - 10.1002/cbic.201500305
Subject(s) - nitrogenase , vanadium , cofactor , chemistry , catalysis , enzyme , cluster (spacecraft) , inorganic chemistry , combinatorial chemistry , organic chemistry , nitrogen fixation , computer science , programming language , nitrogen
Two reaction systems based on vanadium nitrogenase were previously shown to reduce CO 2 to hydrocarbons: 1) an enzyme‐based system that used both components of V nitrogenase for ATP‐dependent reduction of CO 2 to ≤C 2 hydrocarbons; and 2) a cofactor‐based system that employed SmI 2 to supply electrons to the isolated V cluster for an ATP‐independent reduction of CO 2 to ≤C 3 hydrocarbons. Here, we report ATP‐independent reduction of CO 2 to hydrocarbons by a reaction system comprising Eu II DTPA and the VFe protein of V nitrogenase. Combining features of both enzyme‐ and cofactor‐based systems, this system exhibits improved C−C coupling and a broader product profile of ≤C 4 hydrocarbons. The C−C coupling does not employ CO 2 ‐derived CO, and it is significantly enhanced in D 2 O. These observations afford initial insights into the characteristics of this unique reaction and provide a potential template for future design of catalysts to recycle the greenhouse gas CO 2 into useful products.