NDLI: Diiron hexacarbonyl complexes bearing naphthalene-1,8-dithiolate bridge moiety as mimics of the sub-unit of [FeFe]-hydrogenase: synthesis, characterisation and electrochemical investigations

Content Provider	Royal Society of Chemistry (RSC)
Author	Zhong, Wei Liu, Xiaoming Wei, Zhenhong Wang, Hailong Qian, Guifen Xiao, Zhiyin Long, Li
Copyright Year	2015
Abstract	Eight diiron hexacarbonyl complexes bearing a 1,8-dithionaphthalenyl bridging linkage as mimics of the diiron subunit of [FeFe]-hydrogenase are reported. Reaction of Fe3(CO)12 with naphtha[1,8-cd][1,2]dithiole-n-carbaldehyde (n = 2: 2a or 4: 2b) gave two complexes, [Fe2(μ-S)2R(CO)6] (–SRS– = n-formylnaphthalene-1,8-bis(thiolate), n = 2: 3a, 4: 3b), which were further used as precursors to prepare six other complexes by manipulating the formyl groups. Converting the corresponding formyl group into a hydroxymethyl group (CH2OH) led to complexes 4a and 4b. Their reactions with halobutanoyl chloride formed complexes 5a and 5b (halo group = Cl), and 6a and 6b (halo group = Br), respectively. Among the complexes, 3a, 3b, 4b, 5b, and 6a were crystallographically analysed. Electrochemical investigations into these complexes revealed that the formyl group exerts profound electronic influence on the electrochemistry, and thus catalysis of proton reduction, due to its involvement in the conjugation of the bridging linkage. DFT calculations indicate that the formyl group influences the electrochemistry and catalysis by significantly altering the composition of the LUMOs.
Starting Page	9752
Ending Page	9760
Page Count	9
File Format	HTM / HTML PDF
ISSN	11440546
Volume Number	39
Issue Number	12
Journal	New Journal of Chemistry
DOI	10.1039/c5nj02074c
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Hydrogenase Chloride HOMO\/LUMO Triiron dodecacarbonyl SRS Hydrogen Electrochemistry Petroleum naphtha
Content Type	Text
Resource Type	Article
Subject	Chemistry Materials Chemistry Catalysis

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