FullThrOTTLE-TrIR:\nTime-Resolved IR Spectroscopy of\nElectrochemically Generated Species Using a Full Throughput Optically\nTransparent Thin-Layer Electrochemical Cell

An optically transparent thin-layer electrochemical cell\nwith stopped-flow\nsample transport has been developed for optical-pump infrared-probe\ntransient absorption spectroscopy of prereduced or preoxidized molecules.\nTime-resolved IR-spectra of Re(bpy)(CO)<sub>3</sub>X (X = Cl, Br)\ncomplexes in different oxidation states are presented as a proof-of-principle\napplication for this combined electrochemical and spectroscopic tool.\nThe excited-state lifetimes and IR-spectroscopic signatures of various\noxidation states of the molecule, including follow-up reaction intermediates,\nare disentangled by kinetic sorting, using lifetime density analysis.\nThe method can be applied to assign and differentiate molecular intermediates\nin photo- and electrochemical reactions, adding new analytic coordinates\nto classical FTIR- and UV–vis-spectroelectrochemistry.

Publication Details

Journal
Figshare
Published
2024-09-18
DOI
https://doi.org/10.1021/acs.jpcc.4c04947.s001
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
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article

FullThrOTTLE-TrIR:\nTime-Resolved IR Spectroscopy of\nElectrochemically Generated Species Using a Full Throughput Optically\nTransparent Thin-Layer Electrochemical Cell

Figshare
CO2 Reduction Techniques and Catalysts
article

FullThrOTTLE-TrIR:\nTime-Resolved IR Spectroscopy of\nElectrochemically Generated Species Using a Full Throughput Optically\nTransparent Thin-Layer Electrochemical Cell

article en

Abstract

An optically transparent thin-layer electrochemical cell\nwith stopped-flow\nsample transport has been developed for optical-pump infrared-probe\ntransient absorption spectroscopy of prereduced or preoxidized molecules.\nTime-resolved IR-spectra of Re(bpy)(CO)<sub>3</sub>X (X = Cl, Br)\ncomplexes in different oxidation states are presented as a proof-of-principle\napplication for this combined electrochemical and spectroscopic tool.\nThe excited-state lifetimes and IR-spectroscopic signatures of various\noxidation states of the molecule, including follow-up reaction intermediates,\nare disentangled by kinetic sorting, using lifetime density analysis.\nThe method can be applied to assign and differentiate molecular intermediates\nin photo- and electrochemical reactions, adding new analytic coordinates\nto classical FTIR- and UV–vis-spectroelectrochemistry.

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CO2 Reduction Techniques and Catalysts
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