title: A Functional Model of [Fe]-Hydrogenase.
abstract: [Fe]-Hydrogenase catalyzes the hydrogenation of a biological substrate via the heterolytic splitting of molecular hydrogen. While many synthetic models of [Fe]-hydrogenase have been prepared, none yet are capable of activating H2 on their own. Here, we report the first Fe-based functional mimic of the active site of [Fe]-hydrogenase, which was developed based on a mechanistic understanding. The activity of this iron model complex is enabled by its unique ligand environment, consisting of biomimetic pyridinylacyl and carbonyl ligands, as well as a bioinspired diphosphine ligand with a pendant amine moiety. The model complex activates H2 and mediates hydrogenation of an aldehyde.
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Tao
authors.initials: T
authors.lastname: Xu
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Chih-Juo Madeline
authors.initials: CJ
authors.lastname: Yin
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Matthew D
authors.initials: MD
authors.lastname: Wodrich
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Simona
authors.initials: S
authors.lastname: Mazza
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Katherine M
authors.initials: KM
authors.lastname: Schultz
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Rosario
authors.initials: R
authors.lastname: Scopelliti
authors.affiliation: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering and ‡Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) , Lausanne CH-1015, Switzerland.
authors.forename: Xile
authors.initials: X
authors.lastname: Hu
mesh_terms: D000447:Aldehydes / Q000737:chemistry; D040761:Biomimetic Materials / Q000737:chemistry* / Q000378:metabolism; D020134:Catalytic Domain; D056831:Coordination Complexes / Q000737:chemistry*; D041961:Deuterium Exchange Measurement; D006864:Hydrogenase / Q000737:chemistry* / Q000378:metabolism; D058085:Iron Compounds / Q000737:chemistry*; D007506:Iron-Sulfur Proteins / Q000737:chemistry* / Q000378:metabolism; D009682:Magnetic Resonance Spectroscopy; D010720:Phosphines / Q000737:chemistry; D011725:Pyridines / Q000737:chemistry; D013055:Spectrophotometry, Infrared; D013816:Thermodynamics
chemical_list: D000447:Aldehydes; D056831:Coordination Complexes; D058085:Iron Compounds; D007506:Iron-Sulfur Proteins; D010720:Phosphines; D011725:Pyridines; C118830:iron hydrogenase; D006864:Hydrogenase