Effect of Electronic Coupling on Electron Transfer Rates from Photoexcited Naphthalenediimide Radical Anion to Re(bpy)(CO)3X

Martinez, Jose F.; La Porte, Nathan T.; Chaudhuri, Subhajyoti; Sinopoli, Alessandro; Bae, Youn Jue; Sohail, Muhammad; Batista, Victor S.; Wasielewski, Michael R.

doi:10.1021/acs.jpcc.8b12264

Effect of Electronic Coupling on Electron Transfer Rates from Photoexcited Naphthalenediimide Radical Anion to Re(bpy)(CO)₃X

Journal Article · Tue Mar 05 23:00:00 EST 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b12264· OSTI ID:1528916

^[1]; ^[1]; ^[2]; Sinopoli, Alessandro ^[3]; Bae, Youn Jue ^[1]; Sohail, Muhammad ^[3]; ^[1]; ^[1]

Northwestern Univ., Evanston, IL (United States). Center for Light Energy Activated Redox Processes (LEAP), and Inst. for Sustainability and Energy, Dept. of Chemistry
Yale Univ., New Haven, CT (United States). Center for Light Energy Activated Redox Processes (LEAP), and Energy Sciences Inst., Dept. of Chemistry
Hamad Bin Khalifa Univ., Doha (Qatar). Qatar Environment and Energy Research Inst.

The electron transfer rate between a donor and an acceptor depends on the free energy change for the reaction as well as differences in structure and electronic coupling between the initial and final states. Selective excitation of a naphthalenediimide radical anion (NDI•–) covalently linked at the 4-, 5-, or 6-positions of the bipyridine (bpy) in the Re(bpy)(CO)₃X (X = Cl or pyridine) carbon dioxide reduction catalyst results in electron transfer from ^2*NDI^•– to Re(bpy)(CO)₃X to form Re(bpy•–)(CO)₃X, the first intermediate in the photocatalytic reduction of CO₂. Femtosecond UV/vis, near-IR, and mid-IR spectroscopy on these constitutional isomers and a set of appropriate reference molecules show that systematically varying the electronic coupling as well as the reaction free energy increases the lifetime of Re(bpy•–)(CO)₃X by an order of magnitude when the NDI chromophore is attached to the 6-position of bpy. NMR and X-ray structural studies along with computational modeling are used to identify the conformation of Re(6-NDI-bpy)(CO)₃X responsible for these favorable changes. Extending the lifetime of the reduced complex in the covalent photosensitizer–catalyst assembly is a critical requirement for the photocatalytic CO₂ reduction and artificial photosynthesis.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

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

Grant/Contract Number:: FG02-99ER14999; SC0001059

OSTI ID:: 1528916

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 16 Vol. 123; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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