Redox-Active 1D Coordination Polymers of Iron–Sulfur Clusters

Horwitz, Noah E.; Xie, Jiaze; Filatov, Alexander S.; Papoular, Robert J.; Shepard, William E.; Zee, David Z.; Grahn, Mia P.; Gilder, Chloe; Anderson, John S.

doi:10.1021/jacs.8b12339

Title: Redox-Active 1D Coordination Polymers of Iron–Sulfur Clusters

Journal Article · Mon Feb 04 00:00:00 EST 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b12339· OSTI ID:1524597

Horwitz, Noah E. ^[1]; Xie, Jiaze ^[1];

^[1]; Papoular, Robert J. ^[2];

^[3]; Zee, David Z. ^[4]; Grahn, Mia P. ^[1]; Gilder, Chloe ^[1];

^[1]

Univ. of Chicago, Chicago, IL (United States)
Saclay Institute for Matter and Radiation (IRAMIS), Gif-sur-Yvette (France)
Synchrotron SOLEIL, Gif-sur-Yvette (France)
Northwestern Univ., Evanston, IL (United States)

Here we describe the combination of an archetypal redox-active metal sulfide cluster, Fe₄S₄, with an organic linker, 1,4-benzenedithiolate, to prepare coordination polymers containing infinite chains of Fe₄S₄ clusters. The crystal structures of two solid materials have been solved from synchrotron X-ray powder diffraction data using simulated annealing and re-fined by a least-squares Rietveld refinement procedure. The electronic properties of these chains have also been characterized by UV-visible and Mössbauer spectroscopies. Additional experiments demonstrated that these chains can be solubilized by variation of the countercation and that the chain structure is maintained in solution. The redox-activity of the Fe₄S₄ clusters can be accessed with chemical reagents. Introduction of charge carriers by reduction of the Fe₄S₄ clusters is found to increase the electrical conductivity of the materials by up to four orders of magnitude. These results highlight the utility of Fe₄S₄ clusters as redox-active building blocks in preparing new classes of coordination polymers.

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Research Organization:: Univ. of Chicago, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019215

OSTI ID:: 1524597

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 9; Related Information: http://pubs.acs.org/doi/suppl/10.1021/jacs.8b12339/suppl_file/ja8b12339_si_001.pdf; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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