质子化g-C3N4/β-SiC复合材料的制备及光催化降解茜素红性能

doi:10.7503/cjcu20190215

高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (10): 2178.doi: 10.7503/cjcu20190215

质子化g-C₃N₄/β-SiC复合材料的制备及光催化降解茜素红性能

吴之强,刘万毅(),王刚,蔡威,岳晓菲,詹海鹃(),毕淑娴,孟哲,马保军

宁夏大学化学化工学院, 省部共建煤炭高效利用与绿色化工国家重点实验室, 化学国家级实验教学示范中心, 银川 750021

收稿日期:2019-04-12 出版日期:2019-10-10 发布日期:2019-10-16
通讯作者: 刘万毅,詹海鹃 E-mail:liuwy@nxu.edu.cn;zhanhj@nxu.edu.cn
基金资助:
宁夏国内一流学科建设项目(No.NXYLXK2017A04);西部地区建设“一流大学”重大创新项目(No.ZKZD2017003);国家自然科学基金(No.21862013)

Preparation of Protonated g-C₃N₄/β-SiC Composites and Photocatalytic Degradation of Alizarin Red S ^†

WU Zhiqiang,LIU Wanyi(),WANG Gang,CAI Wei,YUE Xiaofei,ZHAN Haijuan(),BI Shuxian,MENG Zhe,MA Baojun

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, National Demonstration Center for Experimental Chemistry Education, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China

Received:2019-04-12 Online:2019-10-10 Published:2019-10-16
Contact: LIU Wanyi,ZHAN Haijuan E-mail:liuwy@nxu.edu.cn;zhanhj@nxu.edu.cn
Supported by:
† Supported by the National First-Rate Discipline Construction of Ningxia, China(No.NXYLXK2017A04);the Major Innovation Projects for Building First-class Universities in China’s Western Region(No.ZKZD2017003);the National Natural Science Foundation of China.(No.21862013)

摘要/Abstract

摘要：

分别采用热解法和溶胶-凝胶-碳热还原法合成了石墨相氮化碳(g-C₃N₄)和纳米级碳化硅(β-SiC), 通过浸渍-热处理法将两者复合并通过浓盐酸质子化, 分别制备了g-C₃N₄/β-SiC和质子化g-C₃N₄/β-SiC(P-g-C₃N₄/β-SiC)复合光催化剂. 利用X射线衍射(XRD)、扫描电子显微镜(SEM)、高分辨透射电子显微镜(HRTEM)、傅里叶变换红外光谱(FTIR)、 X射线光电子能谱(XPS)、紫外-可见漫反射光谱(UV-Vis-DRS)和光致发光光谱(PL)等对样品进行了表征. 结果表明, P-g-C₃N₄/β-SiC复合材料的比表面积增大, 光生电子-空穴对的复合几率降低, 光催化性能明显提高. 在光催化降解染料茜素红(ARS)研究中, 样品的可见光催化活性顺序为P-g-C₃N₄/β-SiC>g-C₃N₄/β-SiC>P-g-C₃N₄>g-C₃N₄>β-SiC. 其中P-g-C₃N₄/β-SiC在60 min内对ARS的降解效率高达99.9%, 符合准一阶动力学模型, 速率常数为0.0967 min ^-1, 且循环使用9次后, 光催化降解效率仍保持97.5%以上.

关键词: g-C₃N₄/β-SiC, 质子化, 光催化降解, 高效循环, 茜素红

Abstract:

Graphite phase carbonitride(g-C₃N₄) and silicon carbide(β-SiC) were synthesized by pyrolysis and sol-gel-carbothermic reduction method, respectively. Then, they were combined by the impregnation-heat treatment and protonated by concentrated hydrochloric acid to prepare g-C₃N₄/β-SiC and protonated g-C₃N₄/β-SiC(P-g-C₃N₄/β-SiC) composite photocatalysts. The samples were analyzed by X-ray diffraction(XRD), scanning electron microscopy(SEM), high resolution transmission electron microscopy(HRTEM), Fourier transform infrared spectroscopy(FTIR), X-ray photoelectron spectroscopy(XPS), UV-Vis diffuse reflectance spectroscopy(UV-Vis-DRS) and phototluminescence(PL) characterization. The results show that the P-g-C₃N₄/β-SiC composite did not retain the lamellar morphology and its specific surface area is significantly increased. The UV-Vis-DRS and PL spectra indicate that the recombination probability of photogenerated electron-hole pairs is significantly reduced, and the band gap is significantly improved. At the same time, experiments revealed that the combination of g-C₃N₄ and β-SiC and protonation can have a positive effect on the effective separation of photogenerated electron-hole pairs. In addition, the catalysts were applied to photocataly-tic degradation of alizarin red S(ARS). The results show that the order of visible light photocatalytic activity of the samples is P-g-C₃N₄/β-SiC>g-C₃N₄/β-SiC>P-g-C₃N₄>g-C₃N₄>β-SiC. The degradation efficiency of sample P-g-C₃N₄/β-SiC to ARS was up to 99.9% within 60 min, which accorded with the pseudo first-order kinetic model. The rate constant was 0.0967 min ^-1. After 9 times of cycle, the photocatalytic degradation efficiency of P-g-C₃N₄/β-SiC for ARS remained above 97.5%.

Key words: g-C₃N₄/β-SiC, Protonation, Photocatalytic degradation, High efficiency cycle, Alizarin red S

中图分类号:

O644.1

TrendMD:

吴之强, 刘万毅, 王刚, 蔡威, 岳晓菲, 詹海鹃, 毕淑娴, 孟哲, 马保军. 质子化g-C₃N₄/β-SiC复合材料的制备及光催化降解茜素红性能. 高等学校化学学报, 2019, 40(10): 2178.

WU Zhiqiang, LIU Wanyi, WANG Gang, CAI Wei, YUE Xiaofei, ZHAN Haijuan, BI Shuxian, MENG Zhe, MA Baojun. Preparation of Protonated g-C₃N₄/β-SiC Composites and Photocatalytic Degradation of Alizarin Red S ^†. Chem. J. Chinese Universities, 2019, 40(10): 2178.

图/表 9

Fig.1 XRD patterns of different materials

Fig.2 SEM images of β-SiC(A), g-C3N4(B), P-g-C3N4(C), g-C3N4/β-SiC(E) and P-g-C3N4/β-SiC(F) and HRTEM image of g-C3N4/β-SiC(D)

Fig.3 FTIR spectra of g-C3N4, P-g-C3N4 and P-g-C3N4/β-SiC

Fig.4 XPS spectra of C1s(A, C) and N1s(B, D) of P-g-C3N4/β-SiC(A, B) and P-g-C3N4(C, D)

Fig.5 UV-Vis-DRS spectra(A) and band gap energy(B) of β-SiC, g-C3N4, g-C3N4/β-SiC, P-g-C3N4 and P-g-C3N4/β-SiC

Fig.6 PL spectra of g-C3N4, g-C3N4/β-Si, P-g-C3N4 and P-g-C3N4/β-SiC

Fig.7 Photodegradation curves(A) and pseudo-first-order kinetics curves(B) of the degradation of ARS by different photocatalysts

Fig.8 Cycling performance of P-g-C3N4/β-SiC for degradation of ARS

Fig.9 Plots of photogenerated carriers trapping in the system of photodegradation of ARS by P-g-C3N4/β-SiC

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质子化g-C₃N₄/β-SiC复合材料的制备及光催化降解茜素红性能

Preparation of Protonated g-C₃N₄/β-SiC Composites and Photocatalytic Degradation of Alizarin Red S ^†

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