Nachimuthu Santhanamoorthi, Shie Wan-Ru, Liaw Der-Jang, Romashko Roman V, Jiang Jyh-Chiang
Department of Chemical Engineering , National Taiwan University of Science and Technology , Taipei 10607 , Taiwan.
Institute of Automation and Control Processes FEB RAS , Vladivostok 690041 , Russia.
J Phys Chem B. 2019 Jun 6;123(22):4735-4744. doi: 10.1021/acs.jpcb.9b00393. Epub 2019 May 23.
We propose a linkage approach by merging ambipolar electrochromic (EC) materials in both π-acceptor-π (π-A-π) and donor-acceptor-donor (D-A-D) configurations and investigated their electrochemical and spectroelectrochemical properties using density functional theory calculations. Here, we considered anthracene, toluene, and pyrene as π-conjugated molecules, triphenylamine (TPA) as a donor, and viologen as an acceptor moiety for π-A-π and D-A-D configurations. We have also explored the substitutional effects in the donor moiety on the overall electrochromism during both oxidation and reduction processes. Here, we mainly focused on the relationship between the structure, substitution of functional groups, electronic and spectral properties, as well as redox potential of the designed monomers. Our calculations indicate that the designed monomers have attractive absorption properties and show clear color switching upon the redox process. We find that the substitution of stronger electron-donating and π-spacer groups create new absorption peaks in the oxidation states. These designed viologen derivatives will be potential candidates, which can be used in both oxidation and reduction processes for upcoming EC devices.
我们提出了一种通过将双极性电致变色（EC）材料合并为π-受体-π（π-A-π）和供体-受体-供体（D-A-D）构型的连接方法，并使用密度泛函理论计算研究了它们的电化学和光谱电化学性质。在这里，我们将蒽、甲苯和芘视为π共轭分子，将三苯胺（TPA）作为供体，将紫精作为π-A-π和D-A-D构型的受体部分。我们还探讨了供体部分的取代效应在氧化和还原过程中对整体电致变色的影响。在这里，我们主要关注所设计单体的结构、官能团取代、电子和光谱性质以及氧化还原电位之间的关系。我们的计算表明，所设计的单体具有吸引人的吸收特性，并且在氧化还原过程中显示出明显的颜色切换。我们发现，更强的供电子和π间隔基团的取代在氧化态下产生了新的吸收峰。这些设计的紫精衍生物将是潜在的候选物，可用于即将到来的EC器件的氧化和还原过程。
