高活性氮化碳纳米片的制备策略

doi:10.3866/PKU.WHXB202008010

Abstract

Abstract:

Layered graphitic carbon nitride (g-C₃N₄) is a typical polymeric semiconductor with an sp² π-conjugated system having great potential in energy conversion, environmental purification, materials science, etc., owing to its unique physicochemical and electrical properties. However, bulk g-C₃N₄ obtained by calcination suffers from a low specific surface area, rapid charge carrier recombination, and poor dispersion in aqueous solutions, which limit its practical applications. Controlling the size of g-C₃N₄ (e.g., preparing g-C₃N₄ nanosheets) can effectively solve the above problems. Compared with the bulk material, g-C₃N₄ nanosheets have a larger specific surface area, richer active sites, and a larger band gap due to the quantum confinement effect. As g-C₃N₄ has a layered structure with strong in-plane C-N covalent bonds and weak van der Waals forces between the layers, g-C₃N₄ nanosheets can be prepared by exfoliating bulk g-C₃N₄. Alternatively, g-C₃N₄ nanosheets can otherwise be obtained through the anisotropic assembly of organic precursors. Nevertheless, some of these methods have various limitations, such as high energy consumption, are time consuming, and have low yield. Accordingly, developing green and cost-effective exfoliation and preparation strategies for g-C₃N₄ nanosheets is necessary. Herein, the research progress of the exfoliation and preparation strategies (including the thermal oxidation etching process, the ultrasound-assisted route, the chemical exfoliation, the mechanical method, and the template method) for two-dimensional C₃N₄ nanosheets are introduced. Their features are systematically analyzed and the perspectives and challenges in the preparation of g-C₃N₄ nanosheets are discussed. This study emphasizes the following: (1) The preparation method of g-C₃N₄ nanosheets should be properly selected according to the practical application needs. Additionally, various strategies (such as chemical method and ultrasonic method) can be combined to exfoliate nanosheets from bulk g-C₃N₄; (2) More reasonable nano- or even subnanostructured g-C₃N₄ nanosheets should be continuously explored; (3) Novel modification strategies, such as defective engineering, heterojunction construction, and surface functional group regulation, should be introduced to improve the reactivity and selectivity of the g-C₃N₄ nanosheets; (4) The application of in situ characterization techniques (such as in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), electron spin resonance (ESR) spectroscopy, and Raman spectroscopy) should also be strengthened to monitor the detailed catalytic process and investigate the g-C₃N₄ nanosheet structure-efficiency relationship. (5) To gain a deeper understanding of the relationship between the macroscopic properties and the microscopic structure, the combination of theoretical calculations and experimental results should be strengthened, which will be beneficial for exploiting high-quality g-C₃N₄ nanosheets.

Key words: Carbon nitride, Nanosheets, Exfoliation, Photocatalysis, Semiconductor

MSC2000:

O649

Kaining Li, Mengxi Zhang, Xiaoyu Ou, Ruina Li, Qin Li, Jiajie Fan, Kangle Lv. Strategies for the Fabrication of 2D Carbon Nitride Nanosheets[J].Acta Phys. -Chim. Sin., 2021, 37(8): 2008010.

Figures/Tables 8

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References 66

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Exfoliated strategies and preparation methods	Advantages	Disadvantages	Scope of application	Ref.
Thermal oxidation etching	Easy to operate	High energy consumption; low yield	Photocatalysis electrocatalysis	30, 40
Ultrasound-assisted method	The obtained nanosheets can inherit the structural characteristics of the bulk C₃N₄ and have fewer defects.	Time consumption	Photocatalysis; electrocatalysis energy storage; bioimaging	41, 42
Chemical exfoliation	The preparation time is relatively short; the obtained samples can be highly dispersed; easy to control the surface charge properties by adjusting the pH value.	Inevitably introduce organic solvents or strong acids; require additional work for removal	Photocatalysis; photosynthesis; Electrocatalysis biomedicine	43-46
Mechanical method	High exfoliated efficiency; simultaneous exfoliation and modification can be achieved	Only obtain small size nanosheets	Photocatalysis; biosensing	47, 48
Template method	Controllable morphology; relatively high yield	Additional additives may affect g-C₃N₄ polymerization; contain unavoidable template removal process	Photocatalysis; energy storage	49-52

Sample	Precursor of bulk g-C₃N₄	Exfoliation method	Thickness (nm)	Surface area (m²·g^-1)	Yield (compared to bulk g-C₃N₄)	Ref.
g-C₃N₄ nanosheets	Dicyandiamide	Thermal oxidation etching	≈ 2	306	6%	40
Porous g-C₃N₄ nanosheets	Thiourea	Thermal exfoliation	16	151	8%	39
Foam-Like holey ultrathin g-C₃N₄ nanosheets	Melamine	Long-time thermal oxidation etching	9.2	277.98	-	53
Ultrathin g-C₃N₄ nanosheets	Melamine	Sonication(in aqueous solution for 16 h)	≈ 2.5	-	-	41
g-C₃N₄ nanosheets	Commercial bulk g-C₃N₄	Sonication (in isopropanol for 10 h)	≈ 2	384	-	54
Monolayer g-C₃N₄ nanosheet	Melamine	Sonication (in mixed solvent for 10 h)	0.38	59.4	-	57
Tri-s-triazine-based crystalline C₃N₄ nanosheets	Melamine	Sonication (in isopropanol for 15 h)	≈ 3.6	203	-	55
Few-layer g-C₃N₄ nanosheets	Melamine	Sonication (in γ-valerolactone for 24 h)	≈ 2	-	-	58
Single atomic layer g-C₃N₄ nanosheet	Dicyandiamide	Chemical exfoliation method(H₂SO₄)	≈ 0.4	205.8	-	43
Amphoteric g-C₃N₄ nanosheets	Melamine	Chemical exfoliation method(H₂SO₄)	≈ 9	-	-	59
g-C₃N₄ nanosheets	Melamine	Chemical exfoliation method(HNO₃)	≈ 1.1	-	-	44
Protonated porous g-C₃N₄ nanosheets	Dicyandiamide	Chemical exfoliation method(H₃PO₄)	≈ 1	55.4	-	60
Ultrathing-C₃N₄ nanoplatelets	Melamine	Ball milling	0.35-0.7	97	15%	47
g-C₃N₄ nanosheets	Dicyandiamide	Ball milling	1.5-20	63.62	-	48
g-C₃N₄ nanosheets	Dicyandiamide	Soft-template	3.1	52.9	-	50
High-crystalline g-C₃N₄ nanosheets	Dicyandiamide	Template method	-	39.24	-	51

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Strategies for the Fabrication of 2D Carbon Nitride Nanosheets

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