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Dicyanobenzothiadiazole (DCBT) Organic Dye as a Visible Light Absorbing Strong Photoinduced Oxidant with a 16 Microsecond Long-Lived Excited State
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2022-11-20 , DOI: 10.1002/aenm.202203102
Qing Yun Li 1 , Leigh Anna Hunt 1 , Kalpani Hirunika Wijesinghe 1 , Christine Curiac 1 , Ashley Williams 1 , Amala Dass 1 , Nathan I. Hammer 1 , Jared H. Delcamp 1
Affiliation  

Strong photoinduced oxidants are important to organic synthesis and solar energy conversion, to chemical fuels or electric. For these applications, visible light absorption is important to solar energy conversion and long-lived excited states are needed to drive catalysis. With respect to these desirable qualities, a series of five 5,6-dicyano[2,1,3]benzothiadiazole (DCBT) dyes are examined as organic chromophores that can serve as strong photooxidants in catalytic systems. The series utilizes a DCBT core with aryl groups on the periphery with varying electron donation strengths relative to the core. The dyes are studied via both steady-state and transient absorption and emission studies. Additionally, computational analysis, voltammetry, crystallography, and absorption spectroelectrochemistry are also used to better understand the behavior of these dyes. Ultimately, a strong photooxidant is arrived at with an exceptionally long excited state lifetime for an organic chromophore of 16 µs. The long-lived excited state photosensitizer is well-suited for use in catalysis, and visible light driven photosensitized water oxidation is demonstrated using a water-soluble photosensitizer.

中文翻译:

二氰基苯并噻二唑 (DCBT) 有机染料作为可见光吸收强光致氧化剂,具有 16 微秒长寿命激发态

强光致氧化剂对于有机合成和太阳能转化为化学燃料或电力很重要。对于这些应用,可见光吸收对于太阳能转换很重要,并且需要长寿命的激发态来驱动催化作用。关于这些理想的品质,研究了一系列五种 5,6-二氰基 [2,1,3] 苯并噻二唑 (DCBT) 染料作为有机发色团,可在催化系统中用作强光氧化剂。该系列采用 DCBT 核心,其外围具有芳基,相对于核心具有不同的电子捐赠强度。通过稳态和瞬态吸收和发射研究来研究染料。此外,计算分析、伏安法、晶体学、和吸收光谱电化学也用于更好地了解这些染料的行为。最终,获得了一种强光氧化剂,其有机发色团的激发态寿命特别长,为 16 µs。长寿命激发态光敏剂非常适合用于催化,并​​且使用水溶性光敏剂证明了可见光驱动的光敏水氧化。
更新日期:2022-11-20
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