Force-modulated reductive elimination from platinum( ii ) diaryl complexes
Abstract
Coupled mechanical forces are known to drive a range of covalent chemical reactions, but the effect of mechanical force applied to a spectator ligand on transition metal reactivity is relatively unexplored. Here we quantify the rate of C(sp2)–C(sp2) reductive elimination from platinum(II) diaryl complexes containing macrocyclic bis(phosphine) ligands as a function of mechanical force applied to these ligands. DFT computations reveal complex dependence of mechanochemical kinetics on the structure of the force-transducing ligand. We validated experimentally the computational finding for the most sensitive of the ligand designs, based on MeOBiphep, by coupling it to a macrocyclic force probe ligand. Consistent with the computations, compressive forces decreased the rate of reductive elimination whereas extension forces increased the rate relative to the strain-free MeOBiphep complex with a 3.4-fold change in rate over a ~290 pN range of restoring forces. The calculated natural bite angle of the free macrocyclic ligand changes with force, but 31P NMR analysis and calculations strongly suggest no significant force-induced perturbation of ground state geometry within the first coordination sphere of the (P–P)PtAr2 complexes. Rather, the force/rate behavior observed across this range of forces is attributed to the coupling of force to the elongation of the O∙∙∙O distance inmore »
- Authors:
-
[2];
[1]
- Department of Chemistry, Duke University, Durham, North Carolina 27708, USA
- Department of Chemistry, University of Liverpool, Crown Street, Liverpool L69 7ZD, UK
- Publication Date:
- Research Org.:
- Duke Univ., Durham, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1810185
- Alternate Identifier(s):
- OSTI ID: 1838999
- Grant/Contract Number:
- SC0018188
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 12 Journal Issue: 33; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Yu, Yichen, Wang, Chenxu, Wang, Liqi, Sun, Cai-Li, Boulatov, Roman, Widenhoefer, Ross A., and Craig, Stephen L. Force-modulated reductive elimination from platinum( ii ) diaryl complexes. United Kingdom: N. p., 2021.
Web. doi:10.1039/D1SC03182A.
Yu, Yichen, Wang, Chenxu, Wang, Liqi, Sun, Cai-Li, Boulatov, Roman, Widenhoefer, Ross A., & Craig, Stephen L. Force-modulated reductive elimination from platinum( ii ) diaryl complexes. United Kingdom. https://doi.org/10.1039/D1SC03182A
Yu, Yichen, Wang, Chenxu, Wang, Liqi, Sun, Cai-Li, Boulatov, Roman, Widenhoefer, Ross A., and Craig, Stephen L. Wed .
"Force-modulated reductive elimination from platinum( ii ) diaryl complexes". United Kingdom. https://doi.org/10.1039/D1SC03182A.
@article{osti_1810185,
title = {Force-modulated reductive elimination from platinum( ii ) diaryl complexes},
author = {Yu, Yichen and Wang, Chenxu and Wang, Liqi and Sun, Cai-Li and Boulatov, Roman and Widenhoefer, Ross A. and Craig, Stephen L.},
abstractNote = {Coupled mechanical forces are known to drive a range of covalent chemical reactions, but the effect of mechanical force applied to a spectator ligand on transition metal reactivity is relatively unexplored. Here we quantify the rate of C(sp2)–C(sp2) reductive elimination from platinum(II) diaryl complexes containing macrocyclic bis(phosphine) ligands as a function of mechanical force applied to these ligands. DFT computations reveal complex dependence of mechanochemical kinetics on the structure of the force-transducing ligand. We validated experimentally the computational finding for the most sensitive of the ligand designs, based on MeOBiphep, by coupling it to a macrocyclic force probe ligand. Consistent with the computations, compressive forces decreased the rate of reductive elimination whereas extension forces increased the rate relative to the strain-free MeOBiphep complex with a 3.4-fold change in rate over a ~290 pN range of restoring forces. The calculated natural bite angle of the free macrocyclic ligand changes with force, but 31P NMR analysis and calculations strongly suggest no significant force-induced perturbation of ground state geometry within the first coordination sphere of the (P–P)PtAr2 complexes. Rather, the force/rate behavior observed across this range of forces is attributed to the coupling of force to the elongation of the O∙∙∙O distance in the transition state for reductive elimination. The results suggest opportunities to experimentally map geometry changes associated with reactions in transition metal complexes and potential strategies for force-modulated catalysis.},
doi = {10.1039/D1SC03182A},
journal = {Chemical Science},
number = 33,
volume = 12,
place = {United Kingdom},
year = {Wed Aug 25 00:00:00 EDT 2021},
month = {Wed Aug 25 00:00:00 EDT 2021}
}
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