原位聚合碳掺杂改性石墨态氮化碳光催化活性研究

doi:10.7517/j.issn.1674-0475.2015.05.434

影像科学与光化学 ›› 2015, Vol. 33 ›› Issue (5): 434-440.DOI: 10.7517/j.issn.1674-0475.2015.05.434

• 论文 • 上一篇

原位聚合碳掺杂改性石墨态氮化碳光催化活性研究

洪星星, 康向东, 刘岗, 成会明

中国科学院金属研究所沈阳材料科学国家(联合)实验室, 辽宁沈阳 110016

收稿日期:2015-07-22 修回日期:2015-07-26 出版日期:2015-09-16 发布日期:2015-09-16
通讯作者: 刘岗
基金资助:
国家重点基础研究发展规划973项目(2014CB239401)和国家自然科学基金项目(51422210)资助

Increasing Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Doping through in situ Polycondensation

HONG Xingxing, KANG Xiangdong, LIU Gang, CHENG Huiming

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, Liaoning, P. R. China

Received:2015-07-22 Revised:2015-07-26 Online:2015-09-16 Published:2015-09-16

摘要/Abstract

摘要：

本文通过在双氰胺前驱体中添加聚乙二醇,在缩聚过程实现碳掺杂形成含氮空位的g-C₃N₄光催化剂。通过X射线衍射(XRD)、红外光谱(FTIR)、光电子能谱(XPS)、紫外-可见吸收光谱(UV-Vis)和荧光谱(FL)等表征手段,考察了原位聚合碳掺杂形成氮空位对g-C₃N₄物相结构、组分与化学态、光吸收性能及光催化活性的影响。研究结果表明,采用该方法可实现原位聚合碳掺杂,有效拓展g-C₃N₄的可见光吸收至850 nm,在紫外-可见光与可见光照射下光降解RhB及光催化产氢性能均显著提高,尤其可见光条件下的性能提升更为显著。

关键词: 光催化, g-C₃N₄, 掺杂, 空位, 聚乙二醇

Abstract:

In this paper, g-C₃N₄ with nitrogen vacancy was obtained by carbon doping during in situ polycondensation process from the mixture of dicyandiamide precursor and polyethylene glycol additive. XRD, FTIR, XPS, UV-Vis and FL spectroscopies were employed to investigate the influence of the nitrogen vacancy on the phase structure, composition and chemical states, the light absorption and photocatalytic activity of the as-prepared g-C₃N₄. The results show that in situ carbon doping in the framework of g-C₃N₄ can effectively extend its visible light absorption range to 850 nm. As a consequence, the nitrogen-deficient g-C₃N₄shows much superior photocatalytic activities compared to the pristine g-C₃N₄ in degrading the organic pollutant Rhodamine B and generating hydrogen from aqueous solution containing triethanolamine scavenger under both UV-visible light and visible light irradiation, especially more prominent under visible light irradiation.

Key words: photocatalysis, g-C₃N₄, doping, vacancy, polyethylene glycol

洪星星, 康向东, 刘岗, 成会明. 原位聚合碳掺杂改性石墨态氮化碳光催化活性研究[J]. 影像科学与光化学, 2015, 33(5): 434-440.

HONG Xingxing, KANG Xiangdong, LIU Gang, CHENG Huiming. Increasing Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Doping through in situ Polycondensation[J]. Imaging Science and Photochemistry, 2015, 33(5): 434-440.

参考文献

[1] Fujishima A, Honda K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature (London),1972,238(5358): 37-38.
[2] Kudo A,Miseki Y. Heterogeneous photocatalyst materials for water splitting[J]. Chemical Society Reviews,2009, 38(1): 253-278.
[3] Wen F Y,Yang J H,Zong X,Ma Y,Xu Q,Ma B J,Li C. Photocatalytic hydrogen production utilizing solar energy[J]. Progress in Chemistry,2009,21(11): 2285-2302.
[4] Wang X, Maeda K, Thomas A, Takanabe K, Xin G, Carlsson J M, Domen K,Antonietti M. A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J]. Nature Materials, 2009, 8(1): 76-80.
[5] Zhang J H, Wang B, Wang X C. Carbon nitride polymeric semiconductor for photocatalysis[J]. Progress in Chemistry,2014, 26(1) : 19-29.
[6] Goettmann F, Fischer A, Antonietti M,Thomas A. Metal-free catalysis of sustainable Friedel-Crafts reactions: direct activation of benzene by carbon nitrides to avoid the use of metal chlorides and halogenated compounds[J]. Chemical Communications,2006, (43): 4530-4532.
[7] Goettmann F, Fischer A, Antonietti M,Thomas A. Chemical synthesis of mesoporous carbon nitrides using hard templates and their use as a metal-free catalyst for Friedel-Crafts reaction of benzene[J]. Angewandte Chemie-International Edition, 2006, 45(27): 4467-4471.
[8] Niu P, Liu G, Cheng H M. Nitrogen vacancy-promoted photocatalytic activity of graphitic carbon nitride[J]. The Journal of Physical Chemistry C,2012, 116(20): 11013-11018.
[9] Niu P, Yin L C, Yang Y Q, Liu G, Cheng H M. Increasing the visible light absorption of graphitic carbon nitride (melon) photocatalysts by homogeneous self-modification with nitrogen vacancies[J]. Advanced Materials,2014, 26(47): 8046-8052.
[10] Tong H, Ouyang S, Bi Y, Umezawa N, Oshikiri M,Ye J. Nano-photocatalytic materials: possibilities and challenges[J]. Advanced Materials,2012, 24(2): 229-251.
[11] Ni M, Leung M K H, Leung D Y C,Sumathy K. A review and recent developments in photocatalytic water-splitting using TiO₂ for hydrogen production[J]. Renewable and Sustainable Energy Reviews,2007,11(3): 401-425.
[12] Thomas A, Fischer A, Goettmann F, Antonietti M, Müller J O, Schlgl R,Carlsson J M. Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts[J]. Journal of Materials Chemistry,2008, 18(41): 4893-4908.
[13] Lotsch B Y, Doeblinger M, Sehnert J, Seyfarth L, Senker J, Oeckler O,Schnick W. Unmasking melon by a complementary approach employing electron diffraction, solid-state NMR spectroscopy, and theoretical calculations-structural characterization of a carbon nitride polymer[J]. Chemistry A Europe Journal,2007, 13(17): 4969-4980.
[14] Bojdys M J, Mueller J O, Antonietti M,Thomas A. Ionothermal synthesis of crystalline, condensed, graphitic carbon nitride[J]. Chemistry A Europe Journal, 2008, 14(27): 8177-8182.
[15] Qiu Y,Gao L. Chemical synthesis of turbostratic carbon nitride, containing C-N crystallites, at atmospheric pressure[J]. Chemical Communications,2003, (18): 2378-2379.

原位聚合碳掺杂改性石墨态氮化碳光催化活性研究

Increasing Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Doping through in situ Polycondensation

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	马逸骅, 陈琳, 杨永珍, 于世平, 苏秀琴. 钆掺杂碳量子点的制备及其双模态成像研究进展[J]. 影像科学与光化学, 2020, 38(5): 763-770.
[2]	李玥, 李红英, 常玉雪, 周宏艳, 于翔. MoS₂/TiO₂纳米管阵列的一步沉积法制备及光电性能研究[J]. 影像科学与光化学, 2018, 36(4): 331-339.
[3]	李玥, 宋育泽, 陶雁忠, 高风仙, 汤宁. CdS/TiO₂复合纳米网的制备及光催化性能研究[J]. 影像科学与光化学, 2018, 36(3): 275-282.
[4]	李玲, 杜云舒, 王璇, 韩建, 王传义. 甲醛气体在ZnO表面光降解的机理研究[J]. 影像科学与光化学, 2018, 36(2): 171-177.
[5]	吴世康. 光催化中表面等离子体与半导体间的电子转移与能量转移[J]. 影像科学与光化学, 2018, 36(1): 1-13.
[6]	邱申保, 王素敏, 王奇观, 尚嘉茵, 张文治, 杨磊, 樊亚茹. 水溶性氮掺杂石墨烯量子点的合成及其对Pb²⁺的选择性识别研究[J]. 影像科学与光化学, 2018, 36(1): 108-116.
[7]	Samuel Lascio, 籍海峰. 磷纳米材料的光学、光电子和光催化应用[J]. 影像科学与光化学, 2017, 35(5): 587-602.
[8]	张庆宝, 刘强. 可见光催化需氧氧化在有机合成中的应用[J]. 影像科学与光化学, 2017, 35(5): 614-625.
[9]	桂梦茜, 俞洋, 朱诚逸, 刘宏芳, 王锋. 基于金属钴配合物的均相光催化还原二氧化碳研究进展[J]. 影像科学与光化学, 2017, 35(5): 649-657.
[10]	彭成云, 陈勇. 苝衍生物光催化氧化硫醚的研究[J]. 影像科学与光化学, 2017, 35(5): 675-685.
[11]	陈文铖, 李振声, 佟庆笑. 不对称刚性扭曲菲并咪唑分子的设计合成及其深蓝电致发光性能研究[J]. 影像科学与光化学, 2017, 35(5): 720-728.
[12]	王毅虎, 张兵, 马铭, 卢伟鹏, 王佳宁, 郭燕川. 紫外光共聚交联制备GelMA/PEGDA水凝胶[J]. 影像科学与光化学, 2017, 35(4): 574-580.
[13]	聂坤, 杨汉培, 孙慧华, 崔素珍, 吴俊明. 新型Fe掺杂钙钛矿型KMgF₃光催化剂制备及性能[J]. 影像科学与光化学, 2017, 35(1): 61-69.
[14]	朱哲欣, 叶美英. 光催化微反应器中水样光催化降解及Cd²⁺在线检测[J]. 影像科学与光化学, 2016, 34(5): 444-451.
[15]	张亚婷, 李可可, 任绍昭, 王黛玉, 周安宁, 邱介山. 金属改性煤基石墨烯复合材料的制备及其光催化性能[J]. 影像科学与光化学, 2016, 34(5): 475-481.