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利用衰减全反射傅里叶变换红外光谱（ATR-FTIR）和密度泛函理论理解聚（3,4-乙撑二氧噻吩）：聚苯乙烯磺酸盐（PEDOT:PSS）的热力学和动力学

Understanding Thermodynamics and Kinetics of PEDOT:PSS Using ATR-FTIR and Density Functional Theory.

作者信息

Rana Devyesh, Biswakarma John, Lustig Steven R

机构信息

Department of Chemical Engineering, Northeastern University, Boston, Massachusetts 02115, United States.

出版信息

ACS Omega. 2024 Aug 30;9(37):38998-39003. doi: 10.1021/acsomega.4c05552. eCollection 2024 Sep 17.

DOI:10.1021/acsomega.4c05552
PMID:39310137
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11411657/
Abstract

This work demonstrates poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) and divinyl sulfone (DVS) cross-linking to form insoluble and porous PEDOT:PSS-DVS hydrogels. We propose a reaction mechanism and demonstrate the kinetics of a PEDOT:PSS modification that prevents PEDOT:PSS dispersibility. PSS and DVS undergo a second-order reaction between the DVS secondary carbocations and PSS oxygen anion to form a PSS-DVS network. The kinetics, from real-time attenuated total reflectance-Fourier transform infrared spectroscopy and density functional theory, reveal a temperature-dependent rate expression with a 1.458 1/s pre-exponential factor and a 2.429 kcal/mol activation energy. Cryogelation, phase separation, and phase inversion methods induce porosity in the PEDOT:PSS-DVS hydrogels with pore sizes ranging from 12 to 121 μm. Most importantly, the porous PEDOT:PSS-DVS hydrogels do not redisperse in solution. The results provide evidence for the reaction mechanism and kinetics of porous nondispersible PEDOT:PSS-DVS hydrogels.

摘要

这项工作展示了聚（3,4-亚乙基二氧噻吩）聚苯乙烯磺酸盐（PEDOT:PSS）与二乙烯基砜（DVS）交联形成不溶性且多孔的PEDOT:PSS-DVS水凝胶。我们提出了一种反应机理，并证明了防止PEDOT:PSS分散性的PEDOT:PSS改性动力学。PSS和DVS在DVS仲碳正离子与PSS氧阴离子之间发生二级反应，形成PSS-DVS网络。通过实时衰减全反射傅里叶变换红外光谱和密度泛函理论得到的动力学结果显示，其温度依赖速率表达式的指前因子为1.458 1/s，活化能为2.429 kcal/mol。冷冻凝胶化、相分离和相转化方法在PEDOT:PSS-DVS水凝胶中诱导出孔径范围为12至121μm的孔隙。最重要的是，多孔PEDOT:PSS-DVS水凝胶在溶液中不会再分散。这些结果为多孔不可分散PEDOT:PSS-DVS水凝胶的反应机理和动力学提供了证据。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/90f4826b5b49/ao4c05552_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/b35b25c34092/ao4c05552_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/8efa7d902d71/ao4c05552_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/66af72898caa/ao4c05552_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/f2eaa5a444b7/ao4c05552_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/ff260680afeb/ao4c05552_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/90f4826b5b49/ao4c05552_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/b35b25c34092/ao4c05552_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/8efa7d902d71/ao4c05552_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/66af72898caa/ao4c05552_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/f2eaa5a444b7/ao4c05552_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/ff260680afeb/ao4c05552_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2c4b/11411657/90f4826b5b49/ao4c05552_0006.jpg

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