有机光催化剂用于太阳能水分解：分子水平和聚集体水平改性

doi:10.3866/PKU.WHXB202211010

Abstract

Abstract:

Photocatalytic water splitting is a green technology for sustainable hydrogen evolution. To improve photon-to-electron conversion efficiency, the design and development of efficient, stable, and full-spectrum responsive photocatalysts has attracted increasing attention. Many different classes of materials can be used to harness solar photons for photocatalysis, each having their advantages and drawbacks. Compared to inorganic semiconductors, organic semiconductors are rich in π electrons and can be readily modified, allowing for facile control of the optic (absorption region and intensity) and electronic (energy structure) properties, as well as mechanistic pathways. However, photogenerated charge carriers cannot be effectively employed owing to subpar charge carrier transport properties, which arise from the low concentration and low mobility of free charge carriers in organic semiconductors. Appropriate changes in the molecular structure of the organic semiconductors can allow for sunlight utilization across the full visible region and even the infrared region. By controlling the nature of stacking, organic photocatalysts with different compositions, dimension (0, 1, 2, 3), size, and crystallographic orientation can be harnessed to increase sunlight utilization and charge separation efficiencies. By optimizing these properties, the overall photoelectric conversion efficiency and hydrogen production efficiency can be improved. However, the mechanisms of redox reactions in organic semiconductor photocatalytic systems remain unclear owing to the complex nature of the processes and difficulties in study design. Herein, the physical and chemical processes of organic semiconductors are discussed from the perspective of light harvesting, photoexcited charge separation, and surface reactions. The preparation methods of organic semiconductor nanostructures are summarized and the progressive development of organic nanostructures for photocatalytic hydrogen evolution is systematically reviewed. Typical organic semiconductor materials, including perylene diimide, porphyrin, phthalocyanine, fullerenes, graphitic carbon nitride (g-C₃N₄), and other conjugated polymers, are highlighted. Moreover, modification strategies for optimizing optical and electrical properties at the molecular or aggregate level are discussed. Element doping or substitution and group functionalization at the molecular level as well as control over morphologies, components, and dimensions at the aggregate level are reviewed to clarify structure/property relationships and further guide photocatalyst design. All the strategies discussed herein focus on enhancing hole and electron separation while suppressing their recombination, thereby improving the photocatalytic performance in evolution hydrogen. Finally, the key challenges and prospects of organic nanomaterials for photocatalytic evolution hydrogen are presented. We particularly focus on the construction of a system to evaluate the reasonable loading of co-catalysts, photocatalyst morphology regulation, and combined in situ characterization and density functional theory calculations in the context of photocatalytic hydrogen production.

Key words: Organic semiconductor, Nanostructure, Photocatalysis, Hydrogen production from water splitting

Wenjie Zhou, Qihang Jing, Jiaxin Li, Yingzhi Chen, Guodong Hao, Lu-Ning Wang. Organic Photocatalysts for Solar Water Splitting: Molecular- and Aggregate-Level Modifications[J]. Acta Phys. -Chim. Sin. 2023, 39(5), 2211010. doi: 10.3866/PKU.WHXB202211010

Figures/Tables 17

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Table 1

Comparison of the following organic nanostructured semiconductor photocatalysts in H2 production activities."

Photocatalyst	Preparation method	Structure and morphology	Photocatalytic hydrogen evolution efficiency	Reference
phosphoric acid substituted perylene diimide (P-PMPDI)	self-assembly	nanosheet	11.7 mmol∙g⁻¹∙h⁻¹	81
3, 4, 9, 10-Perylenetetracarboxylic diimide/g-C₃N₄	self-assembly	nanowire/nanosheet	1.583 μmol in 3 h	82
3, 4, 9, 10-Perylenetetracarboxylic diimide -phthalic	self-assembly	nanosheet	1.1 mmol∙g⁻¹∙h⁻¹	83
4(hydroxyl phenyl) porphyrin (THPP)	self-assembly	nanowire	19.5 mmol∙g⁻¹∙h⁻¹ in 5 h	53
SA-Zn (4-carboxyphenyl) porphyrin	self-assembly	nanorods	3487.3 μmol∙g⁻¹∙h⁻¹	84
In(IIIE) meso-tetraphenylporphine chloride (InTPPE)	self-assembly	nanorods	845.4 μmol∙mg⁻¹∙h⁻¹	85
Zinc phthalocyanine /TiO₂/Pt	solvothermal method	nanoparticles	3448 µmol∙g⁻¹∙h⁻¹	86
C₆₀/CdS	hydrothermal synthesis	nanostructure	1.73 µmol∙g⁻¹∙h⁻¹	87
C₆₀/ WO₃	hydrothermal synthesis	nanoparticles	154 µmol∙g⁻¹∙h⁻¹	88
C₆₀/MoS₂	ball-milling method	nanoparticles	6.89 µmol∙g⁻¹∙h⁻¹	89
C₆₀/g-C₃N₄	ball-milling method	nanosheet	266 µmol∙g⁻¹∙h⁻¹	90
TiO₂/C₆₀-d-CNTs	hydrothermal synthesis	nanoparticles/nanotubes	651 µmol∙g⁻¹∙h⁻¹	91
polymeric CN nanocages	hard-template method	nanosheet (SSA: 32 m²∙g⁻¹)	227.23 µmol∙g⁻¹∙h⁻¹	92
porous crystalline g-C₃N₄	hard-template method	nanosheet (SSA: 15.34 m²∙g⁻¹)	1010 µmol∙g⁻¹∙h⁻¹	93
g-C₃N₄	soft-template method	nanosheet (SSA: 60.6 m²∙g⁻¹)	60.6 µmol∙h⁻¹	94
oxygen-doped g-C₃N₄	template-free method	nanosheet	1062.4 μmol∙g⁻¹∙h⁻¹	95
carbon-doped g-C₃N₄	thermal decomposition	nanoparticles	364.33 μmol∙g⁻¹∙h⁻¹	96
(1, 3, 5-Triazine-2, 4, 6-triyl) tribenzaldehyde-COF	solvothermal method	nanosheet (SSA: 1603 m²∙g⁻¹)	230 μmol∙g⁻¹∙h⁻¹	97
Pt-TCPP-MOFs	solvothermal method	nanosheet (SSA: 570 m²∙g⁻¹)	11320 μmol∙g⁻¹∙h⁻¹	98
diyne-functionalized conjugated microporous polymers	solvothermal method	nanosphere (SSA: 556 m²∙g⁻¹)	104.86 mmol∙g⁻¹∙h⁻¹	99

Table 1

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Organic Photocatalysts for Solar Water Splitting: Molecular- and Aggregate-Level Modifications

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