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FullThrOTTLE-TrIR：使用全通量光学透明薄层电化学池对电化学产生的物种进行时间分辨红外光谱分析。

FullThrOTTLE-TrIR: Time-Resolved IR Spectroscopy of Electrochemically Generated Species Using a Full Throughput Optically Transparent Thin-Layer Electrochemical Cell.

作者信息

Oppelt Kerstin T, Hamm Peter

机构信息

Department of Chemistry, University of Zurich, Zurich 8057, Switzerland.

出版信息

J Phys Chem C Nanomater Interfaces. 2024 Sep 18;128(38):16040-16049. doi: 10.1021/acs.jpcc.4c04947. eCollection 2024 Sep 26.

DOI:10.1021/acs.jpcc.4c04947
PMID:39355012
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11440584/
Abstract

An optically transparent thin-layer electrochemical cell with stopped-flow sample transport has been developed for optical-pump infrared-probe transient absorption spectroscopy of prereduced or preoxidized molecules. Time-resolved IR-spectra of Re(bpy)(CO)X (X = Cl, Br) complexes in different oxidation states are presented as a proof-of-principle application for this combined electrochemical and spectroscopic tool. The excited-state lifetimes and IR-spectroscopic signatures of various oxidation states of the molecule, including follow-up reaction intermediates, are disentangled by kinetic sorting, using lifetime density analysis. The method can be applied to assign and differentiate molecular intermediates in photo- and electrochemical reactions, adding new analytic coordinates to classical FTIR- and UV-vis-spectroelectrochemistry.

摘要

一种具有停流样品传输功能的光学透明薄层电化学池已被开发出来，用于对预还原或预氧化分子进行光泵浦红外探测瞬态吸收光谱研究。作为这种电化学和光谱联用工具的原理验证应用，展示了处于不同氧化态的Re(bpy)(CO)X（X = Cl，Br）配合物的时间分辨红外光谱。利用寿命密度分析，通过动力学排序解开了该分子各种氧化态（包括后续反应中间体）的激发态寿命和红外光谱特征。该方法可用于在光化学反应和电化学反应中对分子中间体进行归属和区分，为经典的傅里叶变换红外光谱和紫外可见光谱电化学增添了新的分析坐标。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/2851451c7e21/jp4c04947_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/ad13e796ba30/jp4c04947_0001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/260b4c4a2d4c/jp4c04947_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/004cc29ed2f4/jp4c04947_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/2851451c7e21/jp4c04947_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/ad13e796ba30/jp4c04947_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/5a5124c42601/jp4c04947_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/af39b6a1a74a/jp4c04947_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/260b4c4a2d4c/jp4c04947_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/004cc29ed2f4/jp4c04947_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0a0a/11440584/2851451c7e21/jp4c04947_0007.jpg

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