Tunable Rh2(II,II) Light Absorbers as Excited State Electron Donors and Acceptors Accessible with Red/Near-IR Irradiation

Whittemore, Tyler; Millet, Agustin; Sayre, Hannah; Xue, Congcong; Dolinar, Brian; White, Eryn; Dunbar, Kim; Turro, Claudia

doi:10.1021/jacs.8b00599

Tunable Rh₂(II,II) Light Absorbers as Excited State Electron Donors and Acceptors Accessible with Red/Near-IR Irradiation

Journal Article · Wed Apr 04 00:00:00 EDT 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b00599· OSTI ID:1430408

^[1]; ^[2]; Sayre, Hannah ^[3]; Xue, Congcong ^[3]; ^[2]; ^[2]; ^[2]; ^[4]

The Ohio State Univ., Columbus, OH (United States). Department of Chemistry and Biochemistry; The Ohio State University
Texas A & M Univ., College Station, TX (United States). Department of Chemistry
The Ohio State Univ., Columbus, OH (United States). Department of Chemistry and Biochemistry
The Ohio State Univ., Columbus, OH (United States). Department of Chemistry and Biochemistry

In this study, a series of dirhodium(II,II) paddlewheeel complexes of the type cis-[Rh₂(μ-DTolF)₂(μ-L)₂][BF₄]₂, where DTolF = N,N'-di(p-tolyl)formamidinate and L = 1,8-naphthyridine (np), 2-(pyridin-2-yl)-1,8-naphthyridine (pynp), 2-(quinolin-2-yl)-1,8-naphthyridine (qnnp), and 2-(1,8-naphthyridin-2-yl)quinoxaline (qxnp), were synthesized and characterized. These molecules feature new tridentate ligands that concomitantly bridge the dirhodium core and cap the axial positions. The complexes absorb light strongly throughout the ultraviolet/visible range and into the near-infrared region and exhibit relatively long-lived triplet excited-state lifetimes. Both the singlet and triplet excited states exhibit metal/ligand-to-ligand charge transfer (ML-LCT) in nature as determined by transient absorption spectroscopy and spectroelectrochemistry measurements. When irradiated with low-energy light, these black dyes are capable of undergoing reversible bimolecular electron transfer both to the electron acceptor methyl viologen and from the electron donor p-phenylenediamine. Photoinduced charge transfer in the latter was inaccessible with previous Rh₂(II,II) complexes. Finally, these results underscore the fact that the excited state of this class of molecules can be readily tuned for electron-transfer reactions upon simple synthetic modification and highlight their potential as excellent candidates for p- and n-type semiconductor applications and for improved harvesting of low-energy light to drive useful photochemical reactions.

View Accepted Manuscript (DOE)

Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; SC0010542; SC0010721

OSTI ID:: 1430408

Alternate ID(s):: OSTI ID: 1434737

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 15 Vol. 140; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Photocatalytic H ₂ production by dirhodium( ii , ii ) photosensitizers with red light Sayre, Hannah J.; Millet, Agustin; Dunbar, Kim R. Chemical Communications, Vol. 54, Issue 60 https://doi.org/10.1039/c8cc03631d	journal	January 2018
Electron injection into titanium dioxide by panchromatic dirhodium photosensitizers with low energy red light Xue, Congcong; Sayre, Hannah J.; Turro, Claudia Chemical Communications, Vol. 55, Issue 70 https://doi.org/10.1039/c9cc04677a	journal	January 2019
Triplet state promoted reaction of SO 2 with H 2 O by competition between proton coupled electron transfer (pcet) and hydrogen atom transfer (hat) processes Anglada, Josep M.; Martins-Costa, Marilia T. C.; Francisco, Joseph S. Physical Chemistry Chemical Physics, Vol. 21, Issue 19 https://doi.org/10.1039/c9cp01105f	journal	January 2019
Unbridged Rh( ii )–Rh( ii ) complexes of N-heterocyclic carbenes and reactions with O ₂ to form dirhodium( μ – η ¹ : η ¹ -O ₂ ) complexes Yi, Xiaofei; Liu, Bin; Chen, Kai Dalton Transactions, Vol. 48, Issue 12 https://doi.org/10.1039/c9dt00421a	journal	January 2019
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