碳纳米球复合g-C<sub>3</sub>N<sub>4</sub>提升光催化降解酸性橙Ⅱ性能

张彩霞; 霍彦廷; 邹来禧; 舒庆

doi:10.13801/j.cnki.fhclxb.20210306.001

碳纳米球复合g-C₃N₄提升光催化降解酸性橙Ⅱ性能

doi: 10.13801/j.cnki.fhclxb.20210306.001

江西理工大学　材料冶金化学学部，赣州 341000

基金项目: 国家自然科学基金(21766009)；江西理工大学清江青年英才支持计划资助项目

详细信息

通讯作者:
舒庆，博士，教授，博士生导师，研究方向为催化功能材料　E-mail：shuqing@jxust.edu.cn

中图分类号: O643.3
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- 被引次数: 0
出版历程
- 收稿日期: 2020-12-01
- 录用日期: 2021-02-12
- 网络出版日期: 2021-03-08
- 刊出日期: 2021-11-01

Improvement of the performance of photocatalytic degradation of acid orange Ⅱ by carbon nanospheres combined with g-C₃N₄

Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou, 341000, China

摘要

摘要: 基于g-C₃N₄构建的异质结光催化材料在降解有毒有害污染物方面体现出优良的效果。本研究通过水热法制备了一系列不同碳纳米球(Carbon nanospheres，CS)添加量的x-CS/g-C₃N₄ (x=4wt%、5wt%和7wt%)复合光催化剂，以氙灯光源模拟可见光，探究了x-CS/g-C₃N₄对酸性橙Ⅱ的光催化降解性能。结果表明：5wt% CS/g-C₃N₄的光催化活性最高，光催化反应150 min，酸性橙Ⅱ的降解率达到95%。表征结果表明，g-C₃N₄与CS具有类似的π-π共轭结构，易发生π-π堆积相互作用而有利于电子跃迁。二者复合后能有效增强g-C₃N₄对可见光的吸收效率，降低其表面/界面处的电荷转移电阻，显著增强载流子的传输能力。x-CS/g-C₃N₄可作为一种有效的可见光催化剂应用于有机染料降解，具有应用前景。
- 碳纳米球 /
- g-C₃N₄ /
- 复合光催化剂 /
- 光催化性能 /
- 酸性橙Ⅱ
Abstract: The heterojunction photocatalytic material constructed with g-C₃N₄ as the matrix shows excellent effects in degrading toxic and harmful pollutants. In this study, a series of x-CS/g-C₃N₄ (x=4wt%, 5wt% and 7wt%) composite photocatalysts with different addition amounts of carbon nanospheres (CS) were prepared by hydrothermal method, and the photocatalytic degradation performance of x-CS/g-C₃N₄ on acid orange II were explored when a xenon lamp was used as a visible light source. The results show that the photocatalytic activity of 5wt% CS/g-C₃N₄ is the highest, and the degradation rate of acid orange II reaches 95% when the photocatalytic reaction is 150 min. The characterization results show that g-C₃N₄ and CS have a similar π-π conjugate structure, and π-π stacking interaction is prone to occur, which is beneficial to electronic transition. The combination of g-C₃N₄ and CS can effectively enhance the absorption efficiency of g-C₃N₄ for visible light, reduce the charge transfer resistance at the surface/interface, and significantly enhance the transport capacity of carriers. x-CS/g-C₃N₄ can be used as an effective visible light catalyst for the degradation of organic dyes and has application prospects.
- carbon nanospheres /
- g-C₃N₄ /
- composite photocatalyst /
- photocatalytic performance /
- acid orange II

HTML全文

图 1 CS和x-CS/g-C₃N₄催化剂的SEM图像

Figure 1. SEM images of g-C₃N₄ and x-CS/g-C₃N₄catalyst ((a) CS; (b) 5wt% CS/g-C₃N₄; (c) 7wt% CS/g-C₃N₄; (d) 4wt% CS/g-C₃N₄)

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图 2 5wt% CS/g-C₃N₄催化剂的TEM图像

Figure 2. TEM images of 5wt% CS/g-C₃N₄ catalyst

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图 3 g-C₃N₄和x-CS/g-C₃N₄催化剂的FTIR图谱 (a),XRD图谱 (b) 和PL图谱 (c)

Figure 3. FTIR spectra (a), XRD spectra (b) and PL spectra (c) of g-C₃N₄ and x-CS/g-C₃N₄

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图 4 5wt% CS/g-C₃N₄催化剂的XPS图谱

Figure 4. XPS spectra of 5wt% CS/g-C₃N₄ catalys

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图 5 g-C₃N₄和x-CS/g-C₃N₄催化剂的吸收光谱图(a)和对应的Tauc’s曲线图(b)

Figure 5. Absorption spectra (a) of g-C₃N₄ and x-CS/g-C₃N₄ and their corresponding Tauc’s plots (b)

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图 6 g-C₃N₄和5wt% CS/g-C₃N₄样品的瞬态光电流图

Figure 6. Transient photocurrents of g-C₃N₄ and 5wt% CS/g-C₃N₄

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图 7 g-C₃N₄和5wt% CS/g-C₃N₄样品的电化学阻抗图谱 (a) 和等效电路图 (b)

Figure 7. EIS Nyquist plots (a) and equivalent circuit (b) of g-C₃N₄ and 5wt% CS/g-C₃N₄

R_s1 and R_s2—Solution resistance; Q, W and C—Constant phase angle element, diffusion impedance and double-layer capacitor; R_ct—Charge transfer resistance

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图 8 g-C₃N₄和x-CS/g-C₃N₄催化剂对酸性橙Ⅱ的光降解活性结果

Figure 8. Photodegradation activity of g-C₃N₄ and x-CS/g-C₃N₄ catalysts for acid orange II

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表 1 g-C₃N₄和x-CS/g-C₃N₄催化剂的比表面积、孔容和孔径值

Table 1. Surface area, pore volume and pore size of g-C₃N₄ and x-CS/g-C₃N₄

Sample	Specific surface area/(m²·g⁻¹)	Pore size/nm	Pore volume/ (cm³·g⁻¹)
g-C₃N₄	10.09	31.04	0.14
4wt% CS/g-C₃N₄	34.41	26.32	0.23
5wt% CS/g-C₃N₄	39.17	28.35	0.27
7wt% CS/g-C₃N₄	48.18	31.87	0.39

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表 2 g-C₃N₄和x-CS/g-C₃N₄催化剂的吸收边和带隙能

Table 2. Absorption edge and bandgap energy of g-C₃N₄ and x-CS/g-C₃N₄ catalyst

Sample	λ_g/nm	E_g/eV
g-C₃N₄	452	2.74
4wt% CS/g-C₃N₄	455	2.72
5wt% CS/g-C₃N₄	457	2.71
7wt% CS/g-C₃N₄	457	2.71
Notes: λ_g—Absorption edge; E_g—Bandgap energy.

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表 3 g-C₃N₄与不同碳量子点材料复合而成的光催化剂的光催化性能比较

Table 3. Comparison of the results for a number of CDs/g-C₃N₄-based nanocomposites

Photocatalyst	Preparation method	Degradation	Light source	Efficiency	[Ref]
5wt% CS/g-C₃N₄	Hydrothermal	Acid Orange II	Xenon lamp (500 W)	95% in 150 min	This study
CQDs/g-C₃N₄	Precipitation	RhB	Xenon lamp (250 W)	95.2% in 210 min	[32]
g-C₃N₄/CDs/AgBr	Precipitation	RhB	Xenon lamp (250 W)	96.0% in 40 min	[33]
g-C₃N₄/C-dots	Hydrothermal	MO	Halide lamp (35 W)	92.0% in 180 min	[34]
Graphene/CQDs/g-C₃N₄ nanosheet	Hydrothermal	MO	Xenon lamp (100 W)	91.1% in 240 min	[35]
SDAg-CQDs/ultrathin g-C₃N₄	Thermo- polymerization	Naproxen	Xenon lamp (350 W)	87.5% in 25 min	[36]
g-C₃N₄/CQDs	Deposition	RhB	Xenon lamp (300 W)	100% in 210 min	[37]
g-C₃N₄/AgCl/CD	Impregnation	MB and RhB	LED lamp (40 W)	100% in 75 min (MB) & 90% in 75 min (RhB)	[38]
CdS/CQDs/g-C₃N₄	Thermal polymerization	MB, RhB, phenol	Xenon lamp (300 W)	70, 95, 60% in 120 min (RhB, MB, phenol, respectively)	[39]
g-C₃N₄/Bi₂WO₆/NCQs	In-situ calcination and hydrothermal	RhB and TC	Xenon lamp (800 W)	95% in 45 min (RhB) & 80% in 60 min (TC)	[40]
Notes: CS—Carbon nanospheres; CQDs—Carbon quantum dots; CDs—Carbon dots, SDAg—Single atom-dispersed silver; NCQs—Nitrogen-doped carbon quantum dots; RhB—Rhodamine B; MO—Methyl orange; MB—Methylene blue; TC—Tetracycline.

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