钒卤代过氧化物酶构象模型分子的设计、合成及仿生催化活性

引用本文: 曹运珠, 魏东明, 任冬雪, 陈晨, 邢永恒, 施展. 钒卤代过氧化物酶构象模型分子的设计、合成及仿生催化活性[J]. 物理化学学报, 2011, 27(03): 539-546. doi: 10.3866/PKU.WHXB20110326 shu

Citation: CAO Yun-Zhu, WEI Dong-Ming, REN Dong-Xue, CHEN Chen, XING Yong-Heng, SHI Zhan. Design, Synthesis and Mimic Catalytic Activity of a Vanadium Haloperoxidase Conformation Model Molecule[J]. Acta Physico-Chimica Sinica, 2011, 27(03): 539-546. doi: 10.3866/PKU.WHXB20110326 shu

钒卤代过氧化物酶构象模型分子的设计、合成及仿生催化活性

曹运珠 ^1, ,
魏东明 ^1, ,
任冬雪 ^1, ,
陈晨 ^1, ,
邢永恒 ^1, ,
施展 ^2,

基金项目:
国家自然科学基金(21071071) (21071071)

大连市教育基金(2009J21DW004) (2009J21DW004)

吉林大学无机合成与制备化学国家重点实验室(2010-15)资助 (2010-15)

摘要:

基于钒卤代过氧化物酶(V-HPOs)活性中心的N、O配位环境及活性中心与氨基酸残基、水分子之间的氢键作用的模拟, 我们设计、合成了两种钒氧配合物: (C₃H₅N₂)₂[(VO)₂(μ₂-C₂O₄)(C₂O₄)₂(H₂O)₂] (1)和(VO₂)₂(μ₂- C₂O₄)(C₂H₄N₂)₂ (2), 并通过X射线单晶衍射方法确定了它们的结构. 晶体结构分析表明上述钒氧配合物的配位环境与(V-HPOs)活性中心十分相似, 且在配合物的三维堆积结构中具有类α-螺旋结构. 溴化反应活性研究发现这些钒氧配合物在仿生催化实验中表现出较高的催化活性.

关键词:

English

Design, Synthesis and Mimic Catalytic Activity of a Vanadium Haloperoxidase Conformation Model Molecule

1.
1. College of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, Liaoning Province, P. R. China;
2. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China
Received Date: 20 October 2010
Available Online: 03 March 2011
Fund Project:
国家自然科学基金(21071071)

大连市教育基金(2009J21DW004)

吉林大学无机合成与制备化学国家重点实验室(2010-15)资助

Abstract:

Based on mimicing the N, O coordination environment of the active center of vanadium haloperoxidase (V-HPOs) and the hydrogen-bond interaction between the active center and amino acid residues or water molecules, we designed and synthesized two kinds of oxidovanadium complexes: (C₃H₅N₂)₂[(VO)₂(μ₂-C₂O₄)(C₂O₄)₂(H₂O)₂] (1) and (VO₂)₂(μ₂- C₂O₄)(C₂H₄N₂)₂ (2). We determined their structures by X-ray single crystal diffraction. The crystal structure analysis indicated that the coordination environments of those oxidovanadium complexes were similar to the active center of vanadium haloperoxidase, and there seemed to be a mimicing α-helix structure in the three-dimensional packing structure of the complexes. Additionally, by studying the bromination reaction activity we found that the oxidovanadium complexes had an upper activity during the mimic catalytic process.

Key words:

1. [1]
  
  (1) Vilter, H. Phytochemistry 1984, 23, 1387.
  (1) Vilter, H. Phytochemistry 1984, 23, 1387.
2. [2]
  (2) Messerschmidt, A.; Wever, R. J. Inorg. Biochem. 1995, 59, 580.(2) Messerschmidt, A.; Wever, R. J. Inorg. Biochem. 1995, 59, 580.
3. [3]
  (3) Messerschmidt, A.; Wever, R. Proc. Natl. Acad. Sci. U. S. A. 1996, 93, 392.(3) Messerschmidt, A.; Wever, R. Proc. Natl. Acad. Sci. U. S. A. 1996, 93, 392.
4. [4]
  (4) Butler, A. Bio-Inorg. Chem. 1998, 2, 279.(4) Butler, A. Bio-Inorg. Chem. 1998, 2, 279.
5. [5]
  (5) Maurya, M. R.; Kumar, A.; Ebel, M.; Rehder, D. Inorg. Chem. 2006, 45, 5924.(5) Maurya, M. R.; Kumar, A.; Ebel, M.; Rehder, D. Inorg. Chem. 2006, 45, 5924.
6. [6]
  (6) Kimblin, C.; Bu, X. H.; Butler, A. Inorg. Chem. 2002, 41, 161.(6) Kimblin, C.; Bu, X. H.; Butler, A. Inorg. Chem. 2002, 41, 161.
7. [7]
  (7) Messerschmidt, A.; Prsde, L.; Wever, R. Biol. Chem. 1997, 378, 309.(7) Messerschmidt, A.; Prsde, L.; Wever, R. Biol. Chem. 1997, 378, 309.
8. [8]
  (8) Wikete, C.; Wu, P. S.; Zampella, G.; De, G. L.; Licini, G.; Rehder, D. Inorg. Chem. 2007, 46, 196.(8) Wikete, C.; Wu, P. S.; Zampella, G.; De, G. L.; Licini, G.; Rehder, D. Inorg. Chem. 2007, 46, 196.
9. [9]
  (9) Maurya, M. R.; Agarwal, S.; Bader, C.; Rehder, D. Eur. J. Inorg. Chem. 2005, 147.(9) Maurya, M. R.; Agarwal, S.; Bader, C.; Rehder, D. Eur. J. Inorg. Chem. 2005, 147.
10. [10]
  (10) Zampella, G.; Fantucci, P.; Pecoraro, V. L.; Gioia, L. D. Inorg. Chem. 2006, 45, 7133.(10) Zampella, G.; Fantucci, P.; Pecoraro, V. L.; Gioia, L. D. Inorg. Chem. 2006, 45, 7133.
11. [11]
  (11) Kanamori, K.; Nishida, K.; Miyata, N.; Okamoto, K. Chem. Lett. 1998, 1267.(11) Kanamori, K.; Nishida, K.; Miyata, N.; Okamoto, K. Chem. Lett. 1998, 1267.
12. [12]
  (12) Hirao, T. Chem. Rev. 1997, 97, 2707.(12) Hirao, T. Chem. Rev. 1997, 97, 2707.
13. [13]
  (13) Plass, W. Coord. Chem. Rev. 2003, 237, 205.(13) Plass, W. Coord. Chem. Rev. 2003, 237, 205.
14. [14]
  (14) Sarmah, S.; Hazarika, P.; Islam, N. S.; Rao, A. V. S.; Ramasarma, T. Mol. Cell. Biochem. 2002, 236, 95.(14) Sarmah, S.; Hazarika, P.; Islam, N. S.; Rao, A. V. S.; Ramasarma, T. Mol. Cell. Biochem. 2002, 236, 95.
15. [15]
  (15) Ver poulos, V.; Priebsch, W.; Fritzsche, M.; Rehder, D. Inorg. Chem. 1993, 32, 1844.(15) Ver poulos, V.; Priebsch, W.; Fritzsche, M.; Rehder, D. Inorg. Chem. 1993, 32, 1844.
16. [16]
  (16) Hamstra, B. J.; Houseman, A. L. P.; Colpas, G. J.; Kampf, J. W.; LoBrutto, R.; Frasch, W. D.; Pecoraro, V. L. Inorg. Chem. 1997, 36, 4866.(16) Hamstra, B. J.; Houseman, A. L. P.; Colpas, G. J.; Kampf, J. W.; LoBrutto, R.; Frasch, W. D.; Pecoraro, V. L. Inorg. Chem. 1997, 36, 4866.
17. [17]
  (17) Butler, A.; Sandy, M. Nature 2009, 460, 848.(17) Butler, A.; Sandy, M. Nature 2009, 460, 848.
18. [18]
  (18) Maurya, M. R.; Khan, A. A.; Azam, A.; Ranjan, S.; Mondal, N.; Kumar, A.; Avecilla, F.; Pessoa, J. C. C. Dalton Trans. 2010, 39, 1345.(18) Maurya, M. R.; Khan, A. A.; Azam, A.; Ranjan, S.; Mondal, N.; Kumar, A.; Avecilla, F.; Pessoa, J. C. C. Dalton Trans. 2010, 39, 1345.
19. [19]
  (19) Li, Z. P.; Xing, Y. H.; Zhang, Y. H.; Bai, F. Y.; Zeng, X. Q.; Ge, M. F. Acta Phys. -Chim. Sin. 2009, 25, 741.(19) Li, Z. P.; Xing, Y. H.; Zhang, Y. H.; Bai, F. Y.; Zeng, X. Q.; Ge, M. F. Acta Phys. -Chim. Sin. 2009, 25, 741.
20. [20]
  [李章朋, 邢永恒, 张元红, 白凤英, 曾小庆, 葛茂发. 物理化学学报, 2009, 25, 741.][李章朋, 邢永恒, 张元红, 白凤英, 曾小庆, 葛茂发. 物理化学学报, 2009, 25, 741.]
21. [21]
  (20) Ahmed, M.; Schwendt, P.; Marek, J.; Siva?k, M. Polyhedron 2004, 23, 655.(20) Ahmed, M.; Schwendt, P.; Marek, J.; Siva?k, M. Polyhedron 2004, 23, 655.
22. [22]
  (21) Weyand, M.; Hecht, H. J.; Kieb, M.; Liaud, M. F.; Vilter, H.; Schomburg, D. J. Mol. Biol. 1999, 293(3), 595.(21) Weyand, M.; Hecht, H. J.; Kieb, M.; Liaud, M. F.; Vilter, H.; Schomburg, D. J. Mol. Biol. 1999, 293(3), 595.
23. [23]
  (22) Sarmah, S.; Kalita, D.; Hazarika, P.; Borah, R.; Islam, N. S. Polyhedron 2004, 23, 1097.(22) Sarmah, S.; Kalita, D.; Hazarika, P.; Borah, R.; Islam, N. S. Polyhedron 2004, 23, 1097.
24. [24]
  (23) Reis, P. M.; Silva, J. A. L.; Silva, J. J. R. F. D.; Pombeiro, A. J. L. Chem. Commun. 2000, 1845.(23) Reis, P. M.; Silva, J. A. L.; Silva, J. J. R. F. D.; Pombeiro, A. J. L. Chem. Commun. 2000, 1845.
25. [25]
  (24) Conte, V.; Bortolini, O.; Carraro, M.; Moro, S. J. Inorg. Biochem. 2000, 80, 41.(24) Conte, V.; Bortolini, O.; Carraro, M.; Moro, S. J. Inorg. Biochem. 2000, 80, 41.
26. [26]
  (25) Colpas, G. J.; Hamstra, B. J.; Kampf, J. W.; Pecoraro, V. L. J. Am. Chem. Soc. 1996, 118, 3469.(25) Colpas, G. J.; Hamstra, B. J.; Kampf, J. W.; Pecoraro, V. L. J. Am. Chem. Soc. 1996, 118, 3469.
27. [27]
  (26) Zampella, G.; Kravitz, J. Y.; Webster, C. E.; Fantucci, P.; Hall, M. B.; Carlson, H. A.; Pecoraro, V. L.; Gioia, L. D. Inorg. Chem. 2004, 43, 4127.
  (26) Zampella, G.; Kravitz, J. Y.; Webster, C. E.; Fantucci, P.; Hall, M. B.; Carlson, H. A.; Pecoraro, V. L.; Gioia, L. D. Inorg. Chem. 2004, 43, 4127.

扫一扫看文章

计量

PDF下载量: 972
文章访问数: 2665
HTML全文浏览量: 24

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

钒卤代过氧化物酶构象模型分子的设计、合成及仿生催化活性

English

Design, Synthesis and Mimic Catalytic Activity of a Vanadium Haloperoxidase Conformation Model Molecule

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

钒卤代过氧化物酶构象模型分子的设计、合成及仿生催化活性

English

Design, Synthesis and Mimic Catalytic Activity of a Vanadium Haloperoxidase Conformation Model Molecule

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

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs