Yang Xiaodong, Zhang Bingjie, Gao Yujing, Liu Chenjing, Li Guoping, Rao Bin, Chu Dake, Yan Ni, Zhang Mingming, He Gang
Key Laboratory of Thermo-Fluid Science and Engineering of Ministry of Education, School of Energy and Power Engineering, Frontier Institute of Science and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi, 710054, P. R. China.
The First Affiliated Hospital of Xi'an Jiaotong University, Xi'an Jiaotong University, Xi'an, Shaanxi, 710054, P. R. China.
Adv Sci (Weinh). 2022 Feb;9(5):e2101652. doi: 10.1002/advs.202101652. Epub 2021 Dec 26.
A series of pyrene or pyrene-o-carborane-appendant selenoviologens (Py-SeV , Py-Cb-SeV ) for enhanced photocatalytic hydrogen evolution reaction (HER) and reduction of alkynes is reported. The efficient photoinduced electron transfer (PET) from electron-rich pyrene-o-carborane heterojunction (Py-Cb) with intramolecular charge transfer (ICT) characteristic to electron-deficient selenoviologen (SeV ) (k = 1.2 × 10 s ) endows the accelerating the generation of selenoviologen radical cation (SeV ) compared with Py-SeV and other derivatives. The electrochromic/electrofluorochromic devices' (ECD and EFCD) measurements and supramolecular assembly/disassembly processes of SeV and cucurbit[8]uril (CB[8]) results show that the PET process can be finely tuned by electrochemical and host-guest chemistry methods. By combination with Pt-NPs catalyst, the Py-Cb-SeV -based system shows high-efficiency visible-light-driven HER and highly selective phenylacetylene reduction due to the efficient PET process.
报道了一系列用于增强光催化析氢反应(HER)和炔烃还原的芘或芘 - 邻碳硼烷连接的硒代紫精(Py - SeV、Py - Cb - SeV)。从具有分子内电荷转移(ICT)特性的富电子芘 - 邻碳硼烷异质结(Py - Cb)到缺电子硒代紫精(SeV)的高效光致电子转移(PET)(k = 1.2×10⁶ s⁻¹),与Py - SeV和其他衍生物相比,加速了硒代紫精自由基阳离子(SeV⁺)的生成。硒代紫精与葫芦[8]脲(CB[8])的电致变色/电致荧光变色器件(ECD和EFCD)测量以及超分子组装/解组装过程结果表明,PET过程可通过电化学和主客体化学方法进行精细调节。通过与Pt - NPs催化剂结合,基于Py - Cb - SeV的体系由于高效的PET过程而表现出高效的可见光驱动HER和高选择性的苯乙炔还原。