基于CdS和CdSe纳米半导体材料的可见光催化二氧化碳还原研究进展

doi:10.3866/PKU.WHXB202008043

Abstract

Abstract:

Carbon dioxide (CO₂) is one of the main greenhouse gases in the atmosphere. The conversion of CO₂ into solar fuels (CO, HCOOH, CH₄, CH₃OH, etc.) using artificial photosynthetic systems is an ideal way to utilize CO₂ as a resource and reduce CO₂ emissions. A typical artificial photosynthetic system is composed of three key components: a photosensitizer (PS) to harvest visible light, a catalyst (C) to catalyze CO₂ or protons into carbon-based fuels or H₂, respectively, and a sacrificial electron donor (SED) to consume the holes generated in the PS. In most cases, the PS and catalyst are two different components of a system. However, some components that possess both light harvesting and redox catalysis functionalities, e.g., nano-semiconductors, are referred to as photocatalysts. During photocatalysis, the PS is typically excited by photons to generate excited electrons. The excited electrons in the PS are transferred to the catalyst to generate a reduced catalyst. The reduced catalyst is used as an active intermediate to perform CO₂ binding and transformation. The PS can be recovered through a reaction with the SED. Nano-semiconductors have been used as photosensitizers and/or photocatalysts in photocatalytic CO₂ reduction systems owing to their excellent photophysical and photochemical properties and photostability. CdS and CdSe nano-semiconductors, such as quantum dots, nanorods, and nanosheets, have been widely used in the construction of photocatalytic CO₂ reduction systems. Systems based on CdS or CdSe nano-semiconductors can be classified into three categories. The first category is systems based on CdS or CdSe photocatalysts. In these systems, CdS or CdSe nano-semiconductors function as photocatalysts to catalyze CO₂ reduction without a co-catalyst under visible-light irradiation. The CO₂ reduction reaction occurs at the surface of the CdS or CdSe nano-semiconductors. The second category is systems based on CdS or CdSe composite photocatalysts. CdS or CdSe nano-semiconductors are combined with functional materials, such as reduced graphene oxide or TiO₂, to prepare composite photocatalysts. These composite photocatalysts are expected to improve the lifetime of the charge separation state and inhibit the photocorrosion of the nano-semiconductors during photocatalysis. The third category is hybrid systems containing a CdS nano-semiconductor and molecular catalysts, such as nickel and cobalt complexes and iron porphyrin. In these hybrid systems, CdS functions as a photosensitizer and the CO₂ reduction reaction occurs at the molecular catalyst. This review article introduces the construction of artificial photosynthetic systems and the photocatalytic mechanism of nano-semiconductors, and summarizes the representative works in the three aforementioned categories of systems. Finally, the challenges of nano-semiconductors for photocatalytic CO₂ reduction are discussed.

Key words: Artificial photosynthesis, CO₂ reduction, CdS nano-semiconductor, CdSe quantum dots, Molecular catalyst

Jin Wu, Jing Liu, Wu Xia, Ying-Yi Ren, Feng Wang. Advances on Photocatalytic CO₂ Reduction Based on CdS and CdSe Nano-Semiconductors[J]. Acta Phys. -Chim. Sin. 2021, 37(5), 2008043. doi: 10.3866/PKU.WHXB202008043

Figures/Tables 5

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Entry	Photocatalyst	Cocatalyst	SED	Solvent	Main Product	Selectivity	Efficiency^a	Ref.
1	CdS	–	TEA	DMF	CO	–	–	25
2	CdS	–	2-propanol	CH₃CN/CH₂Cl₂	HCOOH	80%	–	26
3	CdS	–	CH₃OH	CH₃OH	HCOOCH₃	–	3951.9 μmol∙g⁻¹∙h⁻¹	27
4	CdS	–	–	H₂O	CH₃OH	–	144.5 μmol∙g⁻¹∙h⁻¹	28
5	CdS	–	TEOA	H₂O	CO	–	1.6 μmol∙g⁻¹∙h⁻¹	29
6	CdSe	–	TEA	DMF	CO	95%	7.9 × 10⁵ μmol∙g⁻¹∙h⁻¹	33
7	CdSe/CdS	–	TEA	DMF	CO	96%	4.1 × 10⁵ μmol∙g⁻¹∙h⁻¹	34
8	rGO/CdS	–	–	H₂O vapor	CH₄	–	2.5 μmol∙g⁻¹∙h⁻¹	41
9	CdS/TiO₂	–	–	H₂O	CH₃OH	–	31.9 μmol∙g⁻¹∙h⁻¹	42
10	CdS QDs (doping Ni²⁺)	–	TEOA	H₂O	CO	100%	35^b	43
11	CdSe/TiO₂	–	–	H₂O	CH₄	–	0.6 μmol∙g⁻¹∙h⁻¹	44
12	CdSe/ZIF-8	–	TEOA	CH₃CN	CO	–	3.5 μmol∙g⁻¹∙h⁻¹	45
13	CdS	Co-bipy	TEOA	CH₃CN	CO	87%	844 μmol∙g⁻¹∙h⁻¹	47
14	CdS	C1	TEOA	CH₃CN/H₂O	CO	80%	46.5 μmol∙g⁻¹∙h⁻¹	48
15	CdS	C2	TEOA	CH₃CN/H₂O	CO	3.9%	0.40 ± 0.02 ^b	49
16	CdS	C3	TEOA	CH₃CN/H₂O	CO	10.2%	1.07 ± 0.17 ^b	49
17	CdS	C4	TEOA	CH₃CN/H₂O	CO	92.2%	5.11 ± 0.10 ^b	49
18	CdS	C5	TEOA	H₂O	CO	95%	1380^b	56
19	CdS	C6	TEOA	CH₃CN/H₂O	CO	97%	7.5 μmol∙g⁻¹∙h⁻¹	57
20	CdS/Bi₂S₃	C6	TEOA	CH₃CN/H₂O	CO	–	1.9 × 10³ μmol∙g⁻¹∙h⁻¹	58
21	CdS/UiO-bpy/Co	–	TEOA	CH₃CN	CO	85%	235 μmol∙g⁻¹∙h⁻¹	59

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Advances on Photocatalytic CO₂ Reduction Based on CdS and CdSe Nano-Semiconductors

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