期刊
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
卷 647, 期 6, 页码 618-622出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/zaac.202000353
关键词
Hydrogenase; facile synthesis; aminodiphosphine ligand; X-ray crystallography; electrochemistry
资金
- Natural Science Foundation of Shandong Province [ZR2020MB019]
- Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province [CSPC201904]
- Sichuan Provincial Human Resource and Social Security Department, Sichuan University of Science Engineering [2019RC41, 201710622016, y2019030]
The research focused on the chemical properties of the diiron dithiolato hexacarbonyl complex and explored its potential as a catalyst for hydrogen evolution. By synthesizing new complexes, characterizing them, and conducting electrochemical experiments, the study confirmed the catalytic activity of the complexes for hydrogen evolution.
The chemistry of the diiron dithiolato hexacarbonyl complex Fe-2(mu-edt)(CO)(6) (edt, 1,2-ethanedithiolate) has received special attention, largely because that its structure is similar with the active site of [FeFe]-hydrogenase. In order to enrich the chemistry of complex Fe-2(mu-edt)(CO)(6) and synthesize new hydrogen evolution catalysts, a new route to the diiron dithiolato hexacarbonyl complex Fe-2(mu-edt)(CO)(6) was described. Reaction of Fe-3(CO)(12) and Me3SiSCH2CH2SSiMe3 in the presence of Et3N at 80 degrees C afforded Fe-2(mu-edt)(CO)(6) in 90 % yield. Furthermore, reaction of Fe-2(mu-edt)(CO)(6) and aminodiphosphine ligands (Ph2P)(2)NC6H4R (R=-3-CCH, 4-CCH) produced the new PNP-chelated diiron dithiolato complexes Fe-2(mu-edt)(CO)(4){kappa(2)-(Ph2P)(2)NC6H4R} (1 and 2). All the complexes were characterized by elemental analysis, IR, NMR spectroscopy, and particularly for 1 and 2 by X-ray single diffraction analysis. In addition, the electrochemical results indicated that 1 and 2 could be considered as electrocatalysts for hydrogen evolution reaction.
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