固氮酶活性中心研究五十年

doi:10.3866/PKU.DXHX202310133

Abstract

Abstract: Nitrogenase is a catalyst used by nitrogen-fixing microorganisms to convert atmospheric nitrogen into ammonia at ambient temperature and pressure. The structure of the active site in molybdenum nitrogenase has evolved from Fe₂S₂∙Mo₂O₂ to MoFe₇S₉C(R-Hhomocit)(cys)(his) (H₄homocit = homocitric acid, Hcys = cysteine, Hhis = histidine) through advancements in chemical modeling, spectroscopy, and theoretical calculations, especially for structural biology. This paper provides a comprehensive review of the important achievements in the study of the active site of nitrogenase from a chemical structure perspective over the past fifty years.

Key words: Nitrogenase, MoFe-protein, FeMo-cofactor, Active site

Quanliang Chen, Zhaohui Zhou. Research on the Active Site of Nitrogenase over Fifty Years[J].University Chemistry, 2024, 39(7): 287-293.

References

[1] Burgess, B.K.; Lowe, D. J. Chem. Rev. 1996, 96, 2983.
[2] Smith, B, E.; Richards, R. L.; Newton, W. E. Catalysts for Nitrogen Fixation: Nitrogenases, Relevant Chemical Models and Commercial Processes, 1st ed.; Springer: the Netherlands, 2004.
[3] 厦门大学化学系催化教研室固氮研究组. 厦门大学学报(自然版), 1974, 13, 111.
[4] 中国科学院科福建物质结构研究所固氮研究小组. 科学通报, 1975, 20, 540.
[5] Shah, V. K.; Brill, W. J. Proc. Natl. Acad. Sci. U. S. A. 1977, 74, 3249.
[6] Cramer, S. P.; Hodgson, K. O.; Gillum, W. O.; Mortenson, L. E. J. Am. Chem. Soc. 1978, 100, 3398.
[7] Lu, J. In Nitrogen Fixation; Newton, W. E.; Orme-Johnson, W. H., Eds.; University Press: Baltimore, M. D. USA, 1980; Vol. I, p. 343.
[8] Holm, R. H. Chem. Soc. Rev. 1981, 10, 455.
[9] Zimmerman, R.; Miinck, E.; Brill, W. J.; Shah, V. K.; Henzl, M. T.; Rawlings, J.; Orme-Johnson, W. H. Biochem. Biophys. Acta 1978, 537, 185.
[10] Kurtz, D. M.; McMillan, R. S.; Burgess, B. K.; Mortenson, L. E.; Holm, R. H. Proc. Natl. Acad. Sci. U. S. A. 1979, 76, 4986.
[11] Coucouvanis, D.; Kanatzidis, M. G.; Dunham, W. R.; Hagen, W. R. J. Am. Chem. Soc. 1984, 106, 7998.
[12] 杨奇, 谢钢, 陈三平, 张一凡, 郭培宇, 高胜利. 大学化学, 2015, 30 (6), 33.
[13] Challen, P. R.; Koo, S. K.; Dunham, W. R.; Coucouvanis, D. J. Am. Chem. Soc. 1990, 112, 8606.
[14] Coucouvanis, D.; Challen, P. R.; Koo, S. K.; Davis, W. M.; Butler, W.; Dunham, W. R. Inorg. Chem. 1989, 28, 4181.
[15] Teo, B. K.; Averill, B. A. Biochem. Biophys. Res. Commun. 1979, 88, 1454.
[16] Chen, J.; Christiansen, J.; Tittsworth, R. C.; Hales, B. J.; George, S. J.; Coucouvanis, D.; Carmer, S. P. J. Am. Chem. Soc. 1993, 115, 5509.
[17] Georgiadis, M. M.; Komiya, H.; Chakrabarti, P.; Woo, D.; Kornuc, J. J.; Rees, D. C. Science 1992, 257, 1653.
[18] Kim, J.; Rees, D. C. Science 1992, 257, 1677.
[19] Chan, M. K.; Kim J.; Rees, D. C. Science 1993, 260, 792.
[20] Peters, J. W.; Stowell, M. H. B.; Soltis, S. M.; Finnegan, M. G.; Johnson, M. K.; Rees, D. C. Biochemistry 1997, 36, 1181.
[21] Mayer, S. M.; Lawson, D. M.; Gormal, C. A.; Roe, S. M.; Smith, B. E. J. Mol. Biol. 1999, 292, 871.
[22] Einsle, O.; Tezcan, F. A.; Andrade, S. L.; Schmid, B.; Yoshida, M.; Howard, J. B.; Rees, D. C. Science 2002, 297, 1696.
[23] Schmid, B.; Ribbe, M. W.; Einsle, O.; Yoshida, M.; Thomas, L. M.; Dean, D. R.; Rees, D. C.; Burgess, B. K. Science 2002, 296, 352.
[24] Spatzal, T.; Aksoyoglu, M.; Zhang, L.; Andrade, S. L. A.; Schleicher, E.; Weber, S.; Rees, D. C.; Einsle, O. Science 2011, 334, 940.
[25] Roemelt, M.; Ettenhuber, P.; Hu, Y.; Ribbe, M. W.; Neese, F.; Bergmann, U.; Debeer, S.; Lancaster K. M. Science 2011, 334, 974.
[26] Ludden, P. W.; Shah, V. K.; Roberts, G. P.; Homer, M.; Allen, R.; Paustian, T.; Roll, J.; Chatterjee, R.; Madden, M.; Allen, J.; et al. Molybdenum Enzymes Cofactors and Model Systems; American Chemical Society: Washington, DC, USA, 1993; pp. 196-215.
[27] 陈全亮, 陈洪斌, 曹泽星, 周朝晖, 万惠霖, 李颖, 李季伦. 中国科学, 2014, 44 (12), 1849.
[28] Wang, S. Y.; Jin, W. T.; Chen, H. B.; Zhou, Z. H. Dalton Trans. 2018, 47(22), 7412.
[29] Jin, W. T.; Wang, H. X.; Wang, S. Y.; Dapper, C. H.; Li, X.; Newton, W. E.; Zhou, Z. H.; Cramer, S. P. Inorg. Chem. 2019, 58 (4), 2523.
[30] Deng, L.; Wang, H.; Dapper, C. H.; Newton, W. E.; Shilov, S.; Wang, S. L.; Cramer, S. P.; Zhou, Z. H. Commun. Chem. 2020, 3, 145.
[31] Chen, Q. L.; Wang, H. X.; Cramer, S. P.; Zhou, Z. H. Coord. Chem. Rev. 2024, 505, 215662.
[32] Rehder, D. J. Inorg. Biochem. 2000, 80, 133.
[33] Pessoa, J. C.; Garribba, E.; Santos, M. F.; Santos-Silva, T. Coord. Chem. Rev. 2015, 301, 49.
[34] Harwood, C. S. Anu. Rev. Microbiol. 2020, 74, 247.
[35] Sippel, D.; Einsle O. Nat. Chem. Biol. 2017, 13, 956.
[36] Rohde, M.; Grunau, K.; Einsle, O. Angew. Chem. Int. Ed. 2020, 132, 23833.
[37] Rohde, M.; Laun, K.; Zebger, I.; Stripp, S. T.; Einsle, O. Sci. Adv. 2021, 7, eabg4474.
[38] Chen, C. Y.; Chen, M. L.; Wang, H. X.; Cramer, S. P.; Zhou, Z. H. J. Inorg. Biochem. 2014, 141, 114.

Research on the Active Site of Nitrogenase over Fifty Years

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