Yuchen Qiao, Enting Xu, Yameng Hao, Xuemei Yang, Ming Ni
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引用次数: 0
Abstract
Hydrogen has the potential to serve as a new energy resource, reducing greenhouse gas emissions that contribute to climate change. Natural hydrogenases exhibit impressive catalytic abilities for hydrogen production, but they often lack oxygen tolerance. Oxygen-tolerant hydrogenases can work under oxygen by reacting with oxygen to form inactive states, which can be reactivated to catalytic states by oxygen atom removal. Herein, we synthesized three NiFeSe complexes: (NiSe(CH3)FeCp, NiSe(CH3)FeCp* and NiSe(PhNMe2)FeCp) with features of active sites of [NiFeSe]-H2ases, which are the oxygen-tolerant hydrogenases, and we investigated the influence of electronic and steric factors on the oxygen reaction of these “biomimetic” complexes. In our research, we found that they react with oxygen, forming 1-oxygen species, which is related to the O2-damaged [NiFeSe] active site. Through a comparative analysis of oxygen reactions, we have discovered that electronic factors and steric hindrance on Se play a significant role in determining the oxygen reactivity of NiFe complexes related to hydrogenases’ active sites.
期刊介绍:
Inorganics is an open access journal that covers all aspects of inorganic chemistry research. Topics include but are not limited to: synthesis and characterization of inorganic compounds, complexes and materials structure and bonding in inorganic molecular and solid state compounds spectroscopic, magnetic, physical and chemical properties of inorganic compounds chemical reactivity, physical properties and applications of inorganic compounds and materials mechanisms of inorganic reactions organometallic compounds inorganic cluster chemistry heterogenous and homogeneous catalytic reactions promoted by inorganic compounds thermodynamics and kinetics of significant new and known inorganic compounds supramolecular systems and coordination polymers bio-inorganic chemistry and applications of inorganic compounds in biological systems and medicine environmental and sustainable energy applications of inorganic compounds and materials MD