000184892 001__ 184892
000184892 005__ 20180317093206.0
000184892 0247_ $$2doi$$a10.1002/ejic.201300081
000184892 022__ $$a1434-1948
000184892 02470 $$2ISI$$a000329199900031
000184892 037__ $$aARTICLE
000184892 245__ $$aElectronic Elements Governing the Binding of Small Molecules to a [Fe]-hydrogenase Mimic
000184892 269__ $$a2013
000184892 260__ $$bWiley-Blackwell$$c2013
000184892 336__ $$aJournal Articles
000184892 520__ $$a[Fe]-hydrogenase, one of three types of hydrogenases, activates molecular hydrogen. Here, using DFT computations, we examine the electronic elements governing the binding of small ligands to a recently synthesized [Fe]-hydrogenase biomimic. Computed reaction free energies indicate that anionic species, such as CN- and H-, and acceptors, such as CO, bind favourably with the Fe centre. Ligands such as H2O, CH3CN, and H-2, however, do not bind iron. Protonation of an adjacent thiolate ligand on the mimic significantly increases the energies of ligand binding. Additional computational analysis reveals that the degree of electron donation from the ligand to the mimic correlates strongly with overall binding ability. The results give insights into the electronic elements of iron-small-molecule interaction in these model complexes.
000184892 6531_ $$aBiomimetic chemistry
000184892 6531_ $$aEnzyme models
000184892 6531_ $$aHydrogenase
000184892 6531_ $$aDensity functional calculations
000184892 6531_ $$aLigand effects
000184892 6531_ $$aIron
000184892 700__ $$0245391$$aWodrich, Matthew$$g180925
000184892 700__ $$0242979$$aHu, Xile$$g181278
000184892 773__ $$k22-23$$q3993-3999$$tEuropean Journal of Inorganic Chemistry
000184892 8564_ $$s114126$$uhttps://infoscience.epfl.ch/record/184892/files/SI.pdf$$ySI$$zSI
000184892 8564_ $$s576417$$uhttps://infoscience.epfl.ch/record/184892/files/final.pdf$$yPublisher's version$$zPublisher's version
000184892 909CO $$ooai:infoscience.tind.io:184892$$particle$$pSB
000184892 909C0 $$0252113$$pLSCI$$xU11810
000184892 917Z8 $$x181278
000184892 917Z8 $$x181278
000184892 917Z8 $$x148230
000184892 937__ $$aEPFL-ARTICLE-184892
000184892 973__ $$aEPFL$$rREVIEWED$$sPUBLISHED
000184892 980__ $$aARTICLE