浓硫酸法快速制备质子化g-C3N4纳米带及其紫外光催化降解有机染料研究

doi:10.7503/cjcu20180460

高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (12): 2719.doi: 10.7503/cjcu20180460

浓硫酸法快速制备质子化g-C₃N₄纳米带及其紫外光催化降解有机染料研究

李娇娇, 赵卫峰(), 张改, 马爱洁(), 陈卫星, 周宏伟

西安工业大学材料与化工学院, 西安 710021

收稿日期:2018-06-26 出版日期:2018-12-03 发布日期:2018-09-29
作者简介:
联系人简介: 赵卫峰, 男, 博士, 讲师, 主要从事纳米光电功能材料研究. E-mail: zhaoweifeng@xatu.edu.cn;马爱洁, 女, 博士, 副教授, 主要从事功能高分子材料研究. E-mail: maaijie@xatu.edu.cn
基金资助:
国家自然科学基金(批准号: 61604120, 21501139, 51603164)、陕西省自然科学基础研究计划项目(批准号: 2017ZDJC-22)和陕西省教育厅专项科研计划项目(批准号: 17JK0380)资助.

Facile Preparation of Protonated g-C₃N₄ Nanobelts in Concentrated Sulfuric Acid with Enhanced UV Light Photocatalytic Activity for Photodegradation of Organic Dyes^†

LI Jiaojiao, ZHAO Weifeng^*(), ZHANG Gai, MA Aijie^*(), CHEN Weixing, ZHOU Hongwei

School of Materials and Chemical Engineering, Xi’an Technological University, Xi’an 710021, China

Received:2018-06-26 Online:2018-12-03 Published:2018-09-29
Contact: ZHAO Weifeng,MA Aijie E-mail:zhaoweifeng@xatu.edu.cn;maaijie@xatu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.61604120, 21501139, 51603164), the Natural Science Basic Research Plan of Shaanxi Province, China(No.2017ZDJC-22) and the Special Research Plan of Education Department of Shaanxi Province, China(No.17JK0380).

摘要/Abstract

摘要：

利用浓H₂SO₄(质量分数98%)强的质子化作用与水合放热效应, 实现了石墨相氮化碳(g-C₃N₄)在浓H₂SO₄中的快速剥离, 制备了经浓H₂SO₄质子化改性的g-C₃N₄(g-C₃N₄-H₂SO₄)纳米带. 通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、傅里叶变换红外光谱(FTIR)、紫外-可见漫反射光谱(UV-Vis DRS)和荧光光谱(PL)等对样品进行了表征分析. 结果表明, 所制备的g-C₃N₄纳米带与浓H₂SO₄发生了明显的质子化作用. 相比体相g-C₃N₄, g-C₃N₄-H₂SO₄纳米带禁带宽度明显增大, 光生电子-空穴对复合率有效降低. 以亚甲基蓝为目标污染物, 研究了g-C₃N₄-H₂SO₄纳米带在紫外光下的光催化活性, 结果表明, g-C₃N₄-H₂SO₄纳米带在2 h内对水溶液中MB的降解率可接近100%, 紫外光催化性能明显优于体相g-C₃N₄.

关键词: 石墨相氮化碳, 浓硫酸, 快速剥离, 光催化

Abstract:

Graphitic carbon nitride(g-C₃N₄) nanobelts were prepared by a simple method which involves exfoliating bulk g-C₃N₄ in concentrated H₂SO₄ due to the strong protonation ability and rapid hydration heat effect of 98% H₂SO₄ when mixed with water. The obtained samples were characterized by means of X-ray diffraction(XRD), scanning electron microscopy(SEM), Fourier transform infrared spectroscopy(FTIR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS) and photoluminescence(PL) spectroscopy. The characterization results revealed that a significant protonation occurs between the g-C₃N₄ and H₂SO₄ moleculars, making the band gap of the as-prepared g-C₃N₄-H₂SO₄ nanobelts much larger than that of the bulk g-C₃N₄. Therefore, the UV light adsorption was greatly improved compared to that of bulk g-C₃N₄, and the electron-hole recombination was also reduced after the modification process. Methylene blue(MB) dye was used as the target pollutant to further investigate the UV photoactivity of the g-C₃N₄-H₂SO₄ nanobelt samples. It was found that the protonated nanobelts can decompose almost 100% of MB within 2 h, much superior to the bulk g-C₃N₄ under UV light.

Key words: Graphitic carbon nitride(g-C₃N₄), Concentrated H₂SO₄, Rapid exfoliation, Photocatalysis

中图分类号:

O644

TrendMD:

李娇娇, 赵卫峰, 张改, 马爱洁, 陈卫星, 周宏伟. 浓硫酸法快速制备质子化g-C₃N₄纳米带及其紫外光催化降解有机染料研究. 高等学校化学学报, 2018, 39(12): 2719.

LI Jiaojiao,ZHAO Weifeng,ZHANG Gai,MA Aijie,CHEN Weixing,ZHOU Hongwei. Facile Preparation of Protonated g-C₃N₄ Nanobelts in Concentrated Sulfuric Acid with Enhanced UV Light Photocatalytic Activity for Photodegradation of Organic Dyes^†. Chem. J. Chinese Universities, 2018, 39(12): 2719.

图/表 8

Fig.1 Preparation process of g-C3N4 nanobelts

Fig.2 FTIR spectra of bulk g-C3N4 and the g-C3N4-H2SO4 nanobeltsa. Bulk g-C3N4; b. g-C3N4-10H2SO4;c. g-C3N4-15H2SO4; d. g-C3N4-20H2SO4.

Fig.3 XRD patterns of bulk g-C3N4 and g-C3N4-H2SO4 nanobeltsa. Bulk g-C3N4; b. g-C3N4-10H2SO4;c. g-C3N4-15H2SO4; d. g-C3N4-20H2SO4.

Fig.4 SEM images of bulk g-C3N4(A) and g-C3N4-10H2SO4 nanobelts(B, C) and TEM image of g-C3N4-10H2SO4 nanobelts(D)

Fig.5 UV-Vis diffuse reflection spectra of bulk g-C3N4 and g-C3N4-H2SO4 nanobelts

Fig.6 Photoluminescence spectra of bulk g-C3N4(a) and g-C3N4-10H2SO4 nanobelts(b)

Fig.7 Degradation of MB curves of bulk g-C3N4 and g-C3N4-H2SO4 nanobelts under UV light irradiation

Fig.8 Degradation MB kinetic equation fitting curve of bulk g-C3N4 and g-C3N4-H2SO4 nanobelts

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浓硫酸法快速制备质子化g-C₃N₄纳米带及其紫外光催化降解有机染料研究

Facile Preparation of Protonated g-C₃N₄ Nanobelts in Concentrated Sulfuric Acid with Enhanced UV Light Photocatalytic Activity for Photodegradation of Organic Dyes^†

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