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![Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F55858.jpg&w=3840&q=50)
Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase
Published on: December 4, 2017
Hydrophilic Quaternary Ammonium-Group-Containing [FeFe]-Hydrogenase Models: Synthesis, Structures, and
Li-Cheng Song1,2, Yong-Xiang Wang3, Xu-Kang Xing3
1Department of Chemistry, State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin, 300071, P.R. China. lcsong@nankai.edu.cn.
Abstract:
The first quaternary ammonium-group-containing [FeFe]-hydrogenase models [(μ-PDT)Fe2 (CO)4 {κ2 -(Ph2 P)2 N(CH2 )2 NMe2 BzBr}] (2; PDT=propanedithiolate) and [(μ-PDT)Fe2 (CO)4 {μ-(Ph2 P)2 N(CH2 )2 NMe2 BzBr}] (4) have been prepared by the quaternization of their precursors [(μ-PDT)Fe2 (CO)4 {κ2 -(Ph2 P)2 N(CH2 )2 NMe2 }] (1) and [(μ-PDT)Fe2 (CO)4 {μ-(Ph2 P)2 N(CH2 )2 NMe2 }] (3) with benzyl bromide in high yields. Although new complexes 1-4 have been fully characterized by spectroscopic and X-ray crystallographic studies, the chelated complexes 1 and 2 converted into their bridged isomers 3 and 4 at higher temperatures, thus demonstrating that these bridged isomers are thermodynamically favorable. An electrochemical study on hydrophilic models 2 and 4 in MeCN and MeCN/H2 O as solvents indicates that the reduction potentials are shifted to less-negative potentials as the water content increases. This outcome implies that both 2 and 4 are more easily reduced in the mixed MeCN/H2 O solvent than in MeCN. In addition, hydrophilic models 2 and 4 act as electrocatalysts and achieve higher icat /ip values and turnover numbers (TONs) in MeCN/H2 O as a solvent than in MeCN for the production of hydrogen from the weak acid HOAc.
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