Journal
ADVANCED MATERIALS
Volume 33, Issue 1, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202006274
Keywords
2D materials; conjugate polymers; covalent organic frameworks; donor– acceptor structure; photoelectrochemical water reduction
Categories
Funding
- DFG [CRC 1415, 417590517]
- ERC Consolidator Grant (T2DCP) [819698]
- Coordination Networks: Building Blocks for Functional Systems [SPP 1928]
- EU Graphene Flagship (GrapheneCore3) [881603]
- H2020-MSCA-ITN (ULTIMATE) [813036]
- Center of Advancing Electronics Dresden (cfaed)
- Projekt DEAL
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The synthesis of a novel bithiophene-bridged conjugated polymer for photoelectrochemical water reduction is demonstrated, showing promising properties for efficient charge transfer. The polymer exhibits a wide light-harvesting range, suitable optical energy gap, and high photocurrent density for hydrogen evolution.
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 sp(2)-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 H-2-evolution photocurrent density up to approximate to 7.9 mu A 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 mu A cm(-2)). Density functional theory calculations identify the thiophene units and cyano substituents at the vinylene linkage as active sites for the evolution of H-2.
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