Stable Platinum(IV) Corroles: Synthesis, Molecular Structure, and Room-Temperature Near-IR Phosphorescence
Abstract
A series of stable Pt(IV) corrole complexes with the general formula PtIV[TpXPC](m/p-C6H4CN)(py), where TpXPC3- is the trianion of a tris(p-X-phenyl)corrole and X = CF3, H, and CH3, has been synthesized, affording key physicochemical data on a rare and elusive class of metallocorroles. Single-crystal X-ray structures of two of the complexes revealed very short equatorial Pt-N distances of 1.94-1.97 Å, an axial Pt-C distance of ~2.03 Å, and an axial Pt-N distance of ~2.22 Å. The complexes exhibit Soret maxima at ~430 nm, which are essentially independent of the meso-aryl para substituents, and strong Q bands with the most intense peak at 595-599 nm. The substituent-independent Soret maxima are consistent with an innocent PtIV-corrole3- description for the complexes. The low reduction potentials (-1.45 ± 0.08 V vs saturated calomel reference electrode) also support a highly stable Pt(IV) ground state as opposed to a noninnocent corrole•2- description. The reductions, however, are irreversible, which suggests that they involve concomitant cleavage of the Pt-aryl bond. Unlike Pt(IV) porphyrins, two of the complexes, PtIV[TpXPC](m-C6H4CN)(py) (X = CF3 and CH3), were found to exhibit room-temperature near-IR phosphorescence with emission maxima at 813 and 826 nm, respectively. Finally, the quantum yield of ~0.3% is comparable to thosemore »
- Authors:
-
[2];
[3];
[1]
- Arctic Univ. of Norway, Tromsø (Norway). Dept. of Chemistry
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Graz Univ. of Technology, Graz (Austria). Inst. of Analytical Chemistry and Food Chemistry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); Research Council of Norway
- OSTI Identifier:
- 1493261
- Grant/Contract Number:
- AC02-05CH11231; 262229
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Omega
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2470-1343
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Alemayehu, Abraham B., MCormick, Laura J., Gagnon, Kevin J., Borisov, Sergey M., and Ghosh, Abhik. Stable Platinum(IV) Corroles: Synthesis, Molecular Structure, and Room-Temperature Near-IR Phosphorescence. United States: N. p., 2018.
Web. doi:10.1021/acsomega.8b01149.
Alemayehu, Abraham B., MCormick, Laura J., Gagnon, Kevin J., Borisov, Sergey M., & Ghosh, Abhik. Stable Platinum(IV) Corroles: Synthesis, Molecular Structure, and Room-Temperature Near-IR Phosphorescence. United States. https://doi.org/10.1021/acsomega.8b01149
Alemayehu, Abraham B., MCormick, Laura J., Gagnon, Kevin J., Borisov, Sergey M., and Ghosh, Abhik. Fri .
"Stable Platinum(IV) Corroles: Synthesis, Molecular Structure, and Room-Temperature Near-IR Phosphorescence". United States. https://doi.org/10.1021/acsomega.8b01149. https://www.osti.gov/servlets/purl/1493261.
@article{osti_1493261,
title = {Stable Platinum(IV) Corroles: Synthesis, Molecular Structure, and Room-Temperature Near-IR Phosphorescence},
author = {Alemayehu, Abraham B. and MCormick, Laura J. and Gagnon, Kevin J. and Borisov, Sergey M. and Ghosh, Abhik},
abstractNote = {A series of stable Pt(IV) corrole complexes with the general formula PtIV[TpXPC](m/p-C6H4CN)(py), where TpXPC3- is the trianion of a tris(p-X-phenyl)corrole and X = CF3, H, and CH3, has been synthesized, affording key physicochemical data on a rare and elusive class of metallocorroles. Single-crystal X-ray structures of two of the complexes revealed very short equatorial Pt-N distances of 1.94-1.97 Å, an axial Pt-C distance of ~2.03 Å, and an axial Pt-N distance of ~2.22 Å. The complexes exhibit Soret maxima at ~430 nm, which are essentially independent of the meso-aryl para substituents, and strong Q bands with the most intense peak at 595-599 nm. The substituent-independent Soret maxima are consistent with an innocent PtIV-corrole3- description for the complexes. The low reduction potentials (-1.45 ± 0.08 V vs saturated calomel reference electrode) also support a highly stable Pt(IV) ground state as opposed to a noninnocent corrole•2- description. The reductions, however, are irreversible, which suggests that they involve concomitant cleavage of the Pt-aryl bond. Unlike Pt(IV) porphyrins, two of the complexes, PtIV[TpXPC](m-C6H4CN)(py) (X = CF3 and CH3), were found to exhibit room-temperature near-IR phosphorescence with emission maxima at 813 and 826 nm, respectively. Finally, the quantum yield of ~0.3% is comparable to those observed for six-coordinate Ir(III) corroles.},
doi = {10.1021/acsomega.8b01149},
journal = {ACS Omega},
number = 8,
volume = 3,
place = {United States},
year = {Fri Aug 17 00:00:00 EDT 2018},
month = {Fri Aug 17 00:00:00 EDT 2018}
}
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Figure 1: Current status of Pt−corrole chemistry; the complexes prepared in the course of this study are schematically depicted in blue.
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Works referencing / citing this record:
Ambient-temperature near-IR phosphorescence and potential applications of rhenium-oxo corroles
journal, January 2019
- Borisov, Sergey M.; Einrem, Rune F.; Alemayehu, Abraham B.
- Photochemical & Photobiological Sciences, Vol. 18, Issue 5
Unexpected Molecular Structure of a Putative Rhenium‐Dioxo‐Benzocarbaporphyrin Complex. Implications for the Highest Transition Metal Valence in a Porphyrin‐Type Ligand Environment
journal, October 2019
- Alemayehu, Abraham B.; Vazquez‐Lima, Hugo; Teat, Simon J.
- ChemistryOpen, Vol. 8, Issue 10
Unexpected Molecular Structure of a Putative Rhenium‐Dioxo‐Benzocarbaporphyrin Complex. Implications for the Highest Transition Metal Valence in a Porphyrin‐Type Ligand Environment
journal, October 2019
- Alemayehu, Abraham B.; Vazquez‐Lima, Hugo; Teat, Simon J.
- ChemistryOpen, Vol. 8, Issue 10
Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.