Thiophene-Bridged Donor-Acceptor sp2 -Carbon-Linked 2D Conjugated Polymers as Photocathodes for Water Reduction

Thiophene-Bridged Donor-Acceptor sp2 -Carbon-Linked 2D Conjugated Polymers as Photocathodes for Water Reduction

© 2020 The Authors. Advanced Materials published by Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 1 vom: 19. Jan., Seite e2006274
1. Verfasser: Xu, Shunqi (VerfasserIn)
Weitere Verfasser: Sun, Hanjun, Addicoat, Matthew, Biswal, Bishnu P, He, Fan, Park, SangWook, Paasch, Silvia, Zhang, Tao, Sheng, Wenbo, Brunner, Eike, Hou, Yang, Richter, Marcus, Feng, Xinliang
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2021
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article 2D materials, conjugate polymers covalent organic frameworks donor-acceptor structure photoelectrochemical water reduction
Beschreibung
Zusammenfassung:© 2020 The Authors. Advanced Materials published by Wiley-VCH GmbH.
Photoelectrochemical (PEC) water reduction, converting solar energy into environmentally friendly hydrogen fuel, requires delicate design and synthesis of semiconductors with appropriate bandgaps, suitable energy levels of the frontier orbitals, and high intrinsic charge mobility. In this work, the synthesis of a novel bithiophene-bridged donor-acceptor-based 2D sp2 -carbon-linked conjugated polymer (2D CCP) is demonstrated. The Knoevenagel polymerization between the electron-accepting building block 2,3,8,9,14,15-hexa(4-formylphenyl) diquinoxalino[2,3-a:2',3'-c]phenazine (HATN-6CHO) and the first electron-donating linker 2,2'-([2,2'-bithiophene]-5,5'-diyl)diacetonitrile (ThDAN) provides the 2D CCP-HATNThDAN (2D CCP-Th). Compared with the corresponding biphenyl-bridged 2D CCP-HATN-BDAN (2D CCP-BD), the bithiophene-based 2D CCP-Th exhibits a wide light-harvesting range (up to 674 nm), a optical energy gap (2.04 eV), and highest energy occupied molecular orbital-lowest unoccupied molecular orbital distributions for facilitated charge transfer, which make 2D CCP-Th a promising candidate for PEC water reduction. As a result, 2D CCP-Th presents a superb H2 -evolution photocurrent density up to ≈7.9 µA cm-2 at 0 V versus reversible hydrogen electrode, which is superior to the reported 2D covalent organic frameworks and most carbon nitride materials (0.09-6.0 µA cm-2 ). Density functional theory calculations identify the thiophene units and cyano substituents at the vinylene linkage as active sites for the evolution of H2
Beschreibung:Date Revised 13.10.2024
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202006274