铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)4-可见光催化降解罗丹明B

doi:10.6023/A1105261

化学学报 ›› 2012, Vol. 70 ›› Issue (04): 399-404.DOI: 10.6023/A1105261 上一篇下一篇

研究论文

铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)^4-可见光催化降解罗丹明B

王崇太^a, 华英杰^a, 刘希龙^a, 吴春燕^a, 王会会^a, 赵欣欣^a, 刘晓旸^b

a 海南师范大学化学与化工学院海口 571158;
b 吉林大学化学学院无机合成与制备化学国家重点实验室长春 130012

投稿日期:2011-05-26 修回日期:2011-11-07 发布日期:2011-11-21
通讯作者: 华英杰
基金资助:
国家自然科学基金(Nos. 20963003, 21161007)、海南省重点科技项目(No. 090803)、海南省自然科学基金(No. 509009)、吉林省科技发展计划(No. 20090595)、海南省高等学校科研基金(No. HjKj2011-24)和国家大学生创新性实验计划(No. 101165821).

Visible Photocatalytic Degradation of Rhodamine B Using Keggintype Cr(III)-Substituted Heteropolyanion PW₁₁O₃₉Cr(III)(H₂O)^4-

Wang Chongtai^a, Hua Yingjie^a, Liu Xilong^a, Wu Chunyan^a, Wang Huihui^a, Zhao Xinxin^a, Liu Xiaoyang^b

a School of Chemistry and Chemical Engineering, Hainan Normal University, Haikou 571158;
b State Key Laboratory of Inorganic Synthesis Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012

Received:2011-05-26 Revised:2011-11-07 Published:2011-11-21
Supported by:
Project supported by the Natural Science Foundation of China (Nos. 20963003, 21161007 ), the Key Science and Technology Foundation of Hainan Province, China (No. 090803), the Natural Science Foundation of Hainan Province, China (No. 509009), the Technology Development Program of Jilin Province (No. 20090595), the Science Research Foundation of University of Hainan Province, China (No. HjKj2011-24) and the Innovative Experiment Programs for National College Students (No. 101165821).

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摘要/Abstract

为了利用太阳光能去除水体有机染料污染物, 以Keggin型铬取代杂多阴离子PW₁₁O₃₉Cr(III)(H₂O)^4-.(PW₁₁Cr)为光催化剂, 详细研究在可见光照射下PW₁₁Cr对水体有机染料污染物罗丹明B(RhB)的光催化降解作用, 考察RhB和 PW₁₁Cr初始浓度以及溶液pH对RhB可见光催化降解速率的影响, 并通过可见吸收光谱和荧光发射光谱研究水溶液中 PW₁₁Cr和RhB的相互作用, 提出PW₁₁Cr光催化作用的机理. 实验结果表明, 含有50 μmol·L^-1 PW₁₁Cr和10 μmol·L^-1 RhB的水溶液在200 W可见光下照射120 min, RhB的降解率达到100%, 总有机碳去除率约32%. 在PW₁₁Cr浓度较大和 pH<3.5的酸性条件下, PW₁₁Cr与RhB之间易发生络合, 导致RhB光降解速率变慢, 而PW₁₁Cr浓度为50 μmol·L^-1和溶液接近中性条件下, RhB的光降解速率较快.

关键词: 铬取代杂多阴离子, 均相光催化, 罗丹明B, TOC, 可见光降解

In order to remove aquatic organic dye contaminants utilizing the inexpensive and inexhaustible solar energy, the Keggin-type Cr(III)-substituted heteropolyanion PW₁₁O₃₉Cr(III)(H₂O)^4- (PW₁₁Cr) was used as a photocatalyst. The photocatalytic degradation of rhodamine B (RhB) by PW₁₁Cr under visible light irradiation was investigated in details in this study. At the same time, influences of the initial RhB concentration, the PW₁₁Cr concentration and the solution pH on the photocatalytic degradation rate of RhB were also examined. The interaction between PW₁₁Cr and RhB was scrutinized using visible absorption spectrum and fluorescence emission spectrum. A visible photocatalysis mechanism of PW₁₁Cr for RhB photodegradation was proposed. It was found that 100% of RhB degradation and 32% of TOC removal were reached when the solution containing 50 μmol·L^-1 PW₁₁Cr and 10 μmol·L^-1 RhB was exposed to visible-light irra diation for 120 min. The coordination interaction between PW₁₁Cr and RhB occurs readily at pH<3.5 and a high PW₁₁Cr concentration, which leads to a slow RhB degradation rate. In contrast, the degradation rate of RhB is rapid at the PW₁₁Cr concentration of 50 μmol·L^-1 and near neutral solution.

Key words: Cr(III)-substituted heteropolyanion, homogeneous photocatalysis, rhodamine B, TOC, visible light degradation

引用此文

王崇太, 华英杰, 刘希龙, 吴春燕, 王会会, 赵欣欣, 刘晓旸. 铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)^4-可见光催化降解罗丹明B[J]. 化学学报, 2012, 70(04): 399-404.

Wang Chongtai, Hua Yingjie, Liu Xilong, Wu Chunyan, Wang Huihui, Zhao Xinxin, Liu Xiaoyang. Visible Photocatalytic Degradation of Rhodamine B Using Keggintype Cr(III)-Substituted Heteropolyanion PW₁₁O₃₉Cr(III)(H₂O)^4-[J]. Acta Chimica Sinica, 2012, 70(04): 399-404.

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1 Vinod, K. N.; Puttaswamy, T.; Gowda, K. N. N. J. Mol. Catal. A: Chem. 2009, 298, 66.

2 Ayed, L.; Chaieb, K.; Cheref, A.; Bakhrouf, A. World J. Microbiol. Biotechnol. 2009, 25, 705.

3 Weber, E. J.; Adams, R. L. Environ. Sci. Technol. 1995, 29, 1163.

4 He, Z.; Sun, C.; Yang, S.; Ding, Y.; He, H.; Wang, Z. J. Hazard. Mater. 2009, 162, 1477.

5 Li, L.; Dai, W. K.; Yu, P.; Zhao, J.; Qu, Y. B. J. Chem. Technol. Biotechnol. 2009, 84, 399.

6 Kohtani, S.; Tomohiro, M.; Tokumura, K.; Nakagaki, R. Appl. Catal. B 2005, 58, 265.

7 Chen, C. C.; Zhao, W.; Lei, P. X.; Zhao, J. C.; Serpone, N. Chem. Eur. J. 2004, 10, 1956.

8 Fujishima, A.; Rao, T. N.; Tryk, D. A. J. Photochem. Photobiol. C 2001, 1, 1.

9 Chen, X. B.; Mao, S. S. Chem. Rev. 2007, 107, 2891.

10 Gaya, U. I.; Abdullah, A. H. J. Photochem. Photobiol. C 2008, 9, 1.

11 Sano, T.; Puzenat, E.; Guillard, C.; Geantet, C.; Matsuzawa, S.; Negishi, N. J. Phys. Chem. C 2009, 113, 5535.

12 Huang, H. Y.; Gu, X. T.; Zhou, J. H.; Ji, K.; Liu, H. L.; Feng, Y. Y. Catal. Commun. 2009, 11, 58.

13 Yin, M. C.; Li, Z. S.; Kou, J. H.; Zou, Z. G. Environ. Sci. Technol. 2009, 43, 8361

14 Zhao, D.; Chen, C. C.; Wang, Y. F.; Ma, W. H.; Zhao, J. C.; Rajh, T.; Zang, L. Environ. Sci. Technol. 2008, 42, 308.

15 Ji, K. H.; Jang, D. M.; Cho, Y. J.; Myung, Y.; Kim, H. S.; Kim, Y.; Park, J. J. Phys. Chem. C 2009, 113, 19966.

16 Huang, H. J.; Li, D. Z.; Lin, Q.; Shao, Y.; Chen, W.; Hu, Y.; Chen, Y. B.; Fu, X. Z. J. Phys. Chem. C 2009, 113, 14264.

17 Liu, L. P.; Hensel, J.; Fitzmorris, R. C.; Li, Y. D.; Zhang, J. Z. J. Phys. Chem. Lett. 2010, 1, 155.

18 Tayade, R. J.; Kulkarni, R. G.; Jasra, R. V. Ind. Eng. Chem. Res. 2006, 45, 922.

19 Cropek, D.; Kemme, P. A.; Makarova, O. V.; Chen, L. X.; Rajh, T. J. Phys. Chem. C 2008, 112, 8311.

20 Nolan, N. T.; Seery, M. K.; Pillai, S. C. J. Phys. Chem. C 2009, 113, 16151.

21 Aarthi, T.; Madras, G. Ind. Eng. Chem. Res. 2007, 46, 7.

22 Mylonas, A.; Papaconstantinou, E. J. Photochem. Photobiol. A: Chem. 1996, 94, 77.

23 Kormali, P.; Triantis, T.; Dimotikali, D.; Hiskia, A.; Papaconstantinou, E. Appl. Catal. B: Environ. 2006, 68, 139.

24 Mylonas, A.; Hiskia, A.; Papaconstantinou, E. J. Mol. Catal. A: Chem. 1996, 114, 191.

25 Troupis, A.; Triantis, T. M.; Gkika, E.; Hiskia, A.; Papaconstantinou, E. Appl. Catal. B: Environ. 2009, 86, 98.

26 Hori, H.; Hayakawa, E.; Einaga, H.; Kutsuna, S.; Koike, K.; Ibusuki, T.; Kitagawa, H.; Arakawa, R. Environ. Sci. Technol. 2004, 38, 6118.

27 Hori, H.; Hayakawa, E.; Koike, K.; Einaga, H.; Ibusuki, T. J. Mol. Catal. A: Chem. 2004, 211, 35.

28 Hiskia, A.; Mylonas, A.; Papaconstantinou, E. Chem. Soc. Rev. 2001, 30, 62.

29 Androulaki, E.; Hiskia, A.; Dimotikali, D.; Minero, C.; Calza, P.; Pelizzetti, E.; Papaconstantinou, E. Environ. Sci. Technol. 2000, 34, 2024.

30 Lei, P. X.; Chen, C. C.; Yang, J.; Ma, W. H.; Zhao, J. C.; Zang, L. Environ. Sci. Technol. 2005, 39, 8466.

31 Hori, H.; Yamamoto, A.; Koike, K.; Kutsuna, S.; Murayama, M.; Yoshimoto, A.; Arakawa, R. Appl. Catal. B: Environ. 2008, 82, 58.

32 Hua, Y. J.; Sun, Z. F.; Wang, C. T.; Hua, S. Y.; Zhang, D. S.; Tong, Y. X. Acta Chim. Sinica 2010, 68, 1037 (in Chinese). (华英杰, 孙振范, 王崇太, 华淑艳, 张大帅, 童叶翔, 化学学报, 2010, 68, 1037.)

33 Hori, H.; Ishida, K.; Inoue, N.; Koike, K.; Kutsuna, S. Chemosphere 2011, 82, 1129.

34 Cai, T. J.; Liao, Y. C.; Peng, Z. S.; Long, Y. F.; Wei, Z. Y.; Deng, Q. J. Environ. Sci. 2009, 21, 997.

35 Wang, C. T.; Hua, Y. J.; Li, G. R.; Tong, Y. X.; Li, Y. G. Acta Chim. Sinica 2008, 66, 835 (in Chinese). (王崇太, 华英杰, 李高仁, 童叶翔, 李玉光, 化学学报, 2008, 66, 835.)

36 Rong, C. Y.; Anson, F. C. Inorg. Chem. 1994, 33, 1064.

37 Brevard, C.; Schimpf, R.; Tourné, G. F.; Tourné, C. M. J. Am. Chem. Soc. 1983, 105, 7059.

38 Zonnevijlle, F.; Tourné, C. M.; Tourné, G. F. Inorg. Chem. 1982, 21, 2751.

39 Bridgeman, A. J.; Cavigliasso, G. A. J. Phys. Chem. A 2003, 107, 6613.

40 Toth, J. E.; Anson, F. C. J. Electroanal. Chem. 1988, 256, 361.

41 Toth, J. E.; Anson, F. C. J. Am. Chem. Soc. 1989, 111, 2444.

42 Wang, C. T.; Hua, Y. J.; Tong, Y. X. Electrochim. Acta 2010, 55, 6755.

43 Magueres, P. L.; Hubig, S. M.; Lindeman, S. V.; Veya, P.; Kochi, J. K. J. Am. Chem. Soc. 2000, 122, 10073.

44 Zhang, X. M.; Shan, B. Z.; Bai, Z. P.; You, C. Y. Chem. Mater. 1997, 9, 2687.

45 Zhang, R. L.; Zhu, J. J.; Zhao, G. C. Chem. J. Chin. Univ. 1998, 19, 1363 (in Chinese). (张荣丽, 朱俊杰, 赵广超, 高等学校化学学报, 1998, 19, 1363.)

46 Yu, K.; Yang, S. G.; He, H.; Sun, C.; Gu, C. G.; Ju, Y. M. J. Phys. Chem. A 2009, 113, 10024

47 Rong, C. Y.; Pope, M. T. J. Am. Chem. Soc. 1992, 114, 2932.

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铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)^4-可见光催化降解罗丹明B

Visible Photocatalytic Degradation of Rhodamine B Using Keggintype Cr(III)-Substituted Heteropolyanion PW₁₁O₃₉Cr(III)(H₂O)^4-

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铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)4-可见光催化降解罗丹明B

Visible Photocatalytic Degradation of Rhodamine B Using Keggintype Cr(III)-Substituted Heteropolyanion PW11O39Cr(III)(H2O)4-

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铬取代杂多阴离子PWB11BOB39BCr(III)(HB2BO)^4-可见光催化降解罗丹明B

Visible Photocatalytic Degradation of Rhodamine B Using Keggintype Cr(III)-Substituted Heteropolyanion PW₁₁O₃₉Cr(III)(H₂O)^4-