EDOT-based conjugated polymers accessed via C-H direct arylation for efficient photocatalytic hydrogen production.

Autor: Tan ZR; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn., Xing YQ; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn., Cheng JZ; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn., Zhang G; Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University Tianjin 300072 China., Shen ZQ; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn., Zhang YJ; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn., Liao G; Engineering Research Center of Nano-Geomaterials of Ministry of Education, China University of Geosciences Wuhan 430074 China., Chen L; Department of Chemistry, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University Tianjin 300072 China., Liu SY; Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Department of Chemistry, Jiangxi University of Science and Technology Ganzhou 341000 China chelsy@zju.edu.cn chelsy@jxust.edu.cn.
Jazyk: angličtina
Zdroj: Chemical science [Chem Sci] 2022 Jan 14; Vol. 13 (6), pp. 1725-1733. Date of Electronic Publication: 2022 Jan 14 (Print Publication: 2022).
DOI: 10.1039/d1sc05784g
Abstrakt: 3,4-Ethylene dioxythiophene (EDOT), as a monomer of commercial conductive poly(3,4-ethylene dioxythiophene) (PEDOT), has been facilely incorporated into a series of new π-conjugated polymer-based photocatalysts, i.e. , BSO 2 -EDOT, DBT-EDOT, Py-EDOT and DFB-EDOT, through atom-economic C-H direct arylation polymerization (DArP). The photocatalytic hydrogen production (PHP) test shows that donor-acceptor (D-A)-type BSO 2 -EDOT renders the highest hydrogen evolution rate (HER) among the linear conjugated polymers (CPs) ever reported. A HER up to 0.95 mmol h -1 /6 mg under visible light irradiation and an unprecedented apparent quantum yield of 13.6% at 550 nm are successfully achieved. Note that the photocatalytic activities of the C-H/C-Br coupling-derived EDOT-based CPs are superior to those of their counterparts derived from the classical C-Sn/C-Br Stille coupling, demonstrating that EDOT is a promising electron-rich building block which can be facilely integrated into CP-based photocatalysts. Systematic studies reveal that the enhanced water wettability by the integration of polar BSO 2 with hydrophilic EDOT, the increased electron-donating ability by O-C p-π conjugation, the improved electron transfer by D-A architecture, broad light harvesting, and the nano-sized colloidal character in a H 2 O/NMP mixed solvent rendered BSO 2 -EDOT as one of the best CP photocatalysts toward PHP.
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE