Fe掺杂g-C<sub>3</sub>N<sub>4</sub>的制备及其可见光催化性能

引用本文: 金瑞瑞, 游继光, 张倩, 刘丹, 胡绍争, 桂建舟. Fe掺杂g-C₃N₄的制备及其可见光催化性能[J]. 物理化学学报, 2014, 30(9): 1706-1712. doi: 10.3866/PKU.WHXB201406272 shu

Citation: JIN Rui-Rui, YOU Ji-Guang, ZHANG Qian, LIU Dan, HU Shao-Zheng, GUI Jian-Zhou. Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity[J]. Acta Physico-Chimica Sinica, 2014, 30(9): 1706-1712. doi: 10.3866/PKU.WHXB201406272 shu

Fe掺杂g-C₃N₄的制备及其可见光催化性能

基金项目:
新世纪优秀人才支持计划（NCET-11-1011)

国家自然科学基金（21103077)

辽宁省自然科学基金（201202123）资助项目

摘要:

以硝酸铁和三聚氰胺为原料制备不同含铁量的Fe 掺杂石墨氮化碳（g-C₃N₄）. 采用X 射线衍射光谱（XRD）、紫外-可见（UV-Vis）光谱、傅里叶变换红外（FT-IR）光谱、电感耦合等离子体-原子发射光谱（ICP-AES）、荧光（PL）光谱、X光电子能谱（XPS）等分析手段对制备的催化剂进行了表征. 结果表明，铁以离子形式镶嵌在g-C₃N₄的结构单元中，影响了g-C₃N₄的能带结构，增加了g-C₃N₄对可见光的吸收，降低了光生电子-空穴对的复合几率. 以染料罗丹明B的降解为探针反应系统研究了不同含铁量对g-C₃N₄在可见光下催化性能的影响. 结果表明，m（Fe）/m（g-C₃N₄）=0.14%时，制备的Fe 掺杂g-C₃N₄表现出最佳的光催化性能，120 min 内罗丹明B的降解率高达99.7%，速率常数达到0.026 min^-1，是纯g-C₃N₄的3.2 倍. 以叔丁醇、对苯醌、乙二胺四乙酸二钠为自由基（·OH）、自由基（O₂^-·）和空穴（h_VB⁺）的捕获剂，研究了光催化反应机理.

关键词:

English

Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity

1.
Division of Chemistry, Chemical Engineering and Environment, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China
Received Date: 08 May 2014
Available Online: 29 August 2014
Fund Project:
新世纪优秀人才支持计划（NCET-11-1011)

国家自然科学基金（21103077)

辽宁省自然科学基金（201202123）资助项目

Abstract:

A series of Fe-doped graphitic carbon nitride (g-C₃N₄) photocatalysts were prepared using ferric nitrate and melamine as precursors. X-ray diffraction (XRD), ultraviolet-visible (UV-Vis) spectroscopy, Fouriertransform infrared (FT-IR) spectroscopy, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), photoluminescence (PL) spectrum, and X-ray photoelectron spectroscopy (XPS) were used to identify changes in the characteristics caused by coordination of N atoms in the structural units of g-C₃N₄. The results indicate that embedded Fe³⁺ changed the optical properties, affected the energy band structure, and increased the electron/hole separation rate. The activities of the Fe³⁺-doped g-C₃N₄ catalysts were tested in the photocatalytic degradation of rhodamine B (RhB) under visible light. The degradation rate of RhB over Fe³⁺-doped g-C₃N₄ was 99.7% in 120 min. The rate constant for Fe³⁺-doped g-C₃N₄ was 3.2 times as high as that of pure g-C₃N₄. Disodium ethylenediamine tetraacetate, tert-butyl alcohol, and 1,4-benzoquinone were used as hole (h_VB⁺), hydroxyl radical (·OH), and superoxide radical (O₂^-·) scavengers, respectively, to investigate the possible mechanism.

Key words:

1. [1]
  
  (1) Liu, A. Y.; Cohen, M. L. Science 1989, 245, 841. doi: 10.1126/science.245.4920.841
  (1) Liu, A. Y.; Cohen, M. L. Science 1989, 245, 841. doi: 10.1126/science.245.4920.841
2. [2]
  (2) Teter, D. M.; Hemley, R. J. Science 1996, 271, 53. doi: 10.1126/science.271.5245.53(2) Teter, D. M.; Hemley, R. J. Science 1996, 271, 53. doi: 10.1126/science.271.5245.53
3. [3]
  (3) Wang, X. C.; Maeda, K.; Thomas, A.; Takanabe, K.; Xin, G.; Carlsson, J. M.; Domen, K.; Antonietti, M. Nat. Mater. 2009, 8, 76. doi: 10.1038/nmat2317(3) Wang, X. C.; Maeda, K.; Thomas, A.; Takanabe, K.; Xin, G.; Carlsson, J. M.; Domen, K.; Antonietti, M. Nat. Mater. 2009, 8, 76. doi: 10.1038/nmat2317
4. [4]
  (4) Yan, S. C.; Li, Z. S.; Zou, Z. G. Langmuir 2010, 26, 3894. doi: 10.1021/la904023j(4) Yan, S. C.; Li, Z. S.; Zou, Z. G. Langmuir 2010, 26, 3894. doi: 10.1021/la904023j
5. [5]
  (5) Liu, G.; Niu, P.; Sun, C.; Smith, S. C.; Chen, Z.; Lu, G. Q.; Cheng, H. M. J. Am. Chem. Soc. 2010, 132, 11642. doi: 10.1021/ja103798k(5) Liu, G.; Niu, P.; Sun, C.; Smith, S. C.; Chen, Z.; Lu, G. Q.; Cheng, H. M. J. Am. Chem. Soc. 2010, 132, 11642. doi: 10.1021/ja103798k
6. [6]
  (6) Wang, Y.; Di, Y.; Antonietti, M.; Li, H.; Chen, C.;Wang, X. C. Chem. Mater. 2010, 22, 5119. doi: 10.1021/cm1019102(6) Wang, Y.; Di, Y.; Antonietti, M.; Li, H.; Chen, C.;Wang, X. C. Chem. Mater. 2010, 22, 5119. doi: 10.1021/cm1019102
7. [7]
  (7) Chen, X.; Takanabe, K.; Domen, K.; Hou, Y.; Fu, X.; Antonietti, M. J. Am. Chem. Soc. 2009, 131, 1680. doi: 10.1021/ja809307s(7) Chen, X.; Takanabe, K.; Domen, K.; Hou, Y.; Fu, X.; Antonietti, M. J. Am. Chem. Soc. 2009, 131, 1680. doi: 10.1021/ja809307s
8. [8]
  (8) Di, Y.;Wang, X. C.; Thomas, A.; Antonietti, M. ChemCatChem 2010, 2, 834. doi: 10.1002/cctc.201000057(8) Di, Y.;Wang, X. C.; Thomas, A.; Antonietti, M. ChemCatChem 2010, 2, 834. doi: 10.1002/cctc.201000057
9. [9]
  (9) Yang, Y.; Guo, Y.; Liu, F.; Yuan, X.; Guo, Y.; Zhang, S.; Guo, W.; Huo, M. Appl. Catal. B: Environ. 2013, 142, 828.(9) Yang, Y.; Guo, Y.; Liu, F.; Yuan, X.; Guo, Y.; Zhang, S.; Guo, W.; Huo, M. Appl. Catal. B: Environ. 2013, 142, 828.
10. [10]
  (10) Huang, L.; Xu, H.; Li, Y.; Li, H.; Cheng, X.; Xia, J.; Xu, Y.; Cai, G. Dalton Trans. 2013, 42, 8606. doi: 10.1039/c3dt00115f(10) Huang, L.; Xu, H.; Li, Y.; Li, H.; Cheng, X.; Xia, J.; Xu, Y.; Cai, G. Dalton Trans. 2013, 42, 8606. doi: 10.1039/c3dt00115f
11. [11]
  (11) Zhou, X.; Jin, B.; Chen, R.; Peng, F.; Fang, Y. Mater. Res. Bull. 2013, 48, 1447. doi: 10.1016/j.materresbull.2012.12.038(11) Zhou, X.; Jin, B.; Chen, R.; Peng, F.; Fang, Y. Mater. Res. Bull. 2013, 48, 1447. doi: 10.1016/j.materresbull.2012.12.038
12. [12]
  (12) Li, Q. Y.; Zong, L. L.; Xing, Y. Y.;Wang, X. D.; Yu, L. G.; Yang, J. J. Adv. Mater. 2013, 5, 1316. doi: 10.1166/sam.2013.1589(12) Li, Q. Y.; Zong, L. L.; Xing, Y. Y.;Wang, X. D.; Yu, L. G.; Yang, J. J. Adv. Mater. 2013, 5, 1316. doi: 10.1166/sam.2013.1589
13. [13]
  (13) Huang, L. Y.; Xu, H.; Zhang, R. X.; Cheng, X. N.; Xia, J. X.; Xu, Y. G.; Li, H. M. Appl. Surf. Sci. 2014, 283, 25.(13) Huang, L. Y.; Xu, H.; Zhang, R. X.; Cheng, X. N.; Xia, J. X.; Xu, Y. G.; Li, H. M. Appl. Surf. Sci. 2014, 283, 25.
14. [14]
  (14) Feng, X. P.; Zhang, H.; Hang, Z. S. J. Funct. Mater. Devic. 2012, 18, 214. [冯西平, 张宏, 杭祖圣. 功能材料与器件学报, 2012, 18, 214.](14) Feng, X. P.; Zhang, H.; Hang, Z. S. J. Funct. Mater. Devic. 2012, 18, 214. [冯西平, 张宏, 杭祖圣. 功能材料与器件学报, 2012, 18, 214.]
15. [15]
  (15) Yang, X. H.;Wang, H. J.; Lu, X. F.; Cui, D. L.; Zhang, S. Y. Acta Chimica Sinica 2009, 67, 1166. [杨晓晖, 王红军, 陆希峰, 崔得良, 张树永. 化学学报, 2009, 67, 1166.](15) Yang, X. H.;Wang, H. J.; Lu, X. F.; Cui, D. L.; Zhang, S. Y. Acta Chimica Sinica 2009, 67, 1166. [杨晓晖, 王红军, 陆希峰, 崔得良, 张树永. 化学学报, 2009, 67, 1166.]
16. [16]
  (16) Wang, X. C.; Chen, X. F.; Thomas, A.; Fu, X. Z.; Antonietti, M. Adv. Mater. 2009, 21, 1609. doi: 10.1002/adma.v21:16(16) Wang, X. C.; Chen, X. F.; Thomas, A.; Fu, X. Z.; Antonietti, M. Adv. Mater. 2009, 21, 1609. doi: 10.1002/adma.v21:16
17. [17]
  (17) Tonda, S.; Kumar, S.; Kandula, S.; Shanker, V. J. Mater. Chem. A 2014, 2, 6772. doi: 10.1039/c3ta15358d(17) Tonda, S.; Kumar, S.; Kandula, S.; Shanker, V. J. Mater. Chem. A 2014, 2, 6772. doi: 10.1039/c3ta15358d
18. [18]
  (18) Li, F. B.; Li, X. Z.; Hou, M. F.; Cheah, K.W.; Choy,W. C. H. Appl. Catal. A 2005, 285, 181. doi: 10.1016/j.apcata.2005.02.025(18) Li, F. B.; Li, X. Z.; Hou, M. F.; Cheah, K.W.; Choy,W. C. H. Appl. Catal. A 2005, 285, 181. doi: 10.1016/j.apcata.2005.02.025
19. [19]
  (19) Pan, C. S.; Zhu, Y. F. Environ. Sci. Technol. 2010, 44, 5570.(19) Pan, C. S.; Zhu, Y. F. Environ. Sci. Technol. 2010, 44, 5570.
20. [20]
  (20) Wang, D.; Duan, Y.; Luo, Q.; Li, X.; Bao, L. Desalination 2011, 270, 174. doi: 10.1016/j.desal.2010.11.042(20) Wang, D.; Duan, Y.; Luo, Q.; Li, X.; Bao, L. Desalination 2011, 270, 174. doi: 10.1016/j.desal.2010.11.042
21. [21]
  (21) Wang, X. C.; Chen, X.; Thomas, A.; Fu, X.; Antonietti, M. Adv. Mater. 2009, 21, 1609. doi: 10.1002/adma.v21:16(21) Wang, X. C.; Chen, X.; Thomas, A.; Fu, X.; Antonietti, M. Adv. Mater. 2009, 21, 1609. doi: 10.1002/adma.v21:16
22. [22]
  (22) Bojdys, M. J.; Müller, J. O.; Antonietti, M.; Thomas, A. Chem. Eur. J. 2008, 14, 8177. doi: 10.1002/chem.v14:27(22) Bojdys, M. J.; Müller, J. O.; Antonietti, M.; Thomas, A. Chem. Eur. J. 2008, 14, 8177. doi: 10.1002/chem.v14:27
23. [23]
  (23) Li, X. F.; Zhang, J.; Shen, L. H.; Ma, Y. M.; Lei,W.W.; Cui, Q. L.; Zou, G. T. Appl. Phys. A 2009, 94, 387. doi: 10.1007/s00339-008-4816-4(23) Li, X. F.; Zhang, J.; Shen, L. H.; Ma, Y. M.; Lei,W.W.; Cui, Q. L.; Zou, G. T. Appl. Phys. A 2009, 94, 387. doi: 10.1007/s00339-008-4816-4
24. [24]
  (24) Anandan, S.; Kathiravan, K.; Murugesan, V.; Ikuma, Y. Catal. Commun. 2009, 10, 1014. doi: 10.1016/j.catcom.2008.12.054(24) Anandan, S.; Kathiravan, K.; Murugesan, V.; Ikuma, Y. Catal. Commun. 2009, 10, 1014. doi: 10.1016/j.catcom.2008.12.054
25. [25]
  (25) Ge, L.; Han, C. Appl. Catal. B: Environ 2012, 117, 268.(25) Ge, L.; Han, C. Appl. Catal. B: Environ 2012, 117, 268.
26. [26]
  (26) Garade, A. C.; Bharadwaj, M.; Bhagwat, S. V.; Athawale, A. A.; Rode, C. V. Catal. Commun. 2009, 10, 485. doi: 10.1016/j.catcom.2008.10.044(26) Garade, A. C.; Bharadwaj, M.; Bhagwat, S. V.; Athawale, A. A.; Rode, C. V. Catal. Commun. 2009, 10, 485. doi: 10.1016/j.catcom.2008.10.044
27. [27]
  (27) Park, Y.; Kim, J. H.; Lee, K. T.; Jeon, K. Adv. Mater. 2009, 21, 4467. doi: 10.1002/adma.v21:44(27) Park, Y.; Kim, J. H.; Lee, K. T.; Jeon, K. Adv. Mater. 2009, 21, 4467. doi: 10.1002/adma.v21:44
28. [28]
  (28) Cong, Y.; Zhang, J.; Chen, F.; Anpo, M. J. Phys. Chem. C 2007, 111, 6976. doi: 10.1021/jp0685030(28) Cong, Y.; Zhang, J.; Chen, F.; Anpo, M. J. Phys. Chem. C 2007, 111, 6976. doi: 10.1021/jp0685030
29. [29]
  (29) Li, X. Y.;Wang, D. S.; Cheng, G. X.; Luo, Q. Z.; An, J.;Wang, Y. H. Appl. Catal. B: Environ 2008, 81, 267. doi: 10.1016/j.apcatb.2007.12.022(29) Li, X. Y.;Wang, D. S.; Cheng, G. X.; Luo, Q. Z.; An, J.;Wang, Y. H. Appl. Catal. B: Environ 2008, 81, 267. doi: 10.1016/j.apcatb.2007.12.022
30. [30]
  (30) Liu, G.; Niu, P.; Yin, L. C.; Cheng, H. M. J. Am. Chem. Soc. 2012, 134, 9070. doi: 10.1021/ja302897b(30) Liu, G.; Niu, P.; Yin, L. C.; Cheng, H. M. J. Am. Chem. Soc. 2012, 134, 9070. doi: 10.1021/ja302897b
31. [31]
  (31) Zhang, S. Q.; Yang, Y. X.; Guo, Y. N.; Guo,W.;Wang, M.; Guo, Y. H.; Huo, M. X. J. Hazard. Mater. 2013, 261, 235. doi: 10.1016/j.jhazmat.2013.07.025
  (31) Zhang, S. Q.; Yang, Y. X.; Guo, Y. N.; Guo,W.;Wang, M.; Guo, Y. H.; Huo, M. X. J. Hazard. Mater. 2013, 261, 235. doi: 10.1016/j.jhazmat.2013.07.025

扫一扫看文章

计量

PDF下载量: 881
文章访问数: 1086
HTML全文浏览量: 44

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Fe掺杂g-C₃N₄的制备及其可见光催化性能

English

Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Fe掺杂g-C3N4的制备及其可见光催化性能

English

Preparation of Fe-Doped Graphitic Carbon Nitride with Enhanced Visible-Light Photocatalytic Activity

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Fe掺杂g-C₃N₄的制备及其可见光催化性能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs