Nitrogenase reaction represents a major source of the usable form of nitrogen that supports the existence of human population. As such, understanding how small building blocks are assembled into a functional nitrogenase entity is of significant relevance to human health. Using combined genetic, biochemical, spectroscopic and structural approaches, we propose to investigate how M-cluster, the active center of molybdenum nitrogenase, is assembled. Specifically, we will examine the formation of a Fe-S core of M-cluster, the maturation of Fe-S core into an M-cluster, and the transfer of M-cluster from the assembly site to its target location in great detail. Through our proposed studies, we expect to refine the biosynthetic pathway of M-cluster, which will provide crucial insights into th structural-functional relationship of nitrogenase and the general assembly mechanism of complex metal clusters in biological systems.
Using combined genetic, biochemical, spectroscopic and structural approaches, we propose to investigate how M-cluster, the active center of molybdenum nitrogenase, is assembled. Through our proposed studies, we expect to refine the biosynthetic mechanism of M-cluster, which will provide crucial insights into the structural-functional relationship of nitrogenase and the general assembly scheme of complex metal clusters in biological systems.
| Rettberg, Lee A; Wilcoxen, Jarett; Lee, Chi Chung et al. (2018) Probing the coordination and function of Fe4S4 modules in nitrogenase assembly protein NifB. Nat Commun 9:2824 |
| Tanifuji, Kazuki; Lee, Chi Chung; Sickerman, Nathaniel S et al. (2018) Tracing the 'ninth sulfur' of the nitrogenase cofactor via a semi-synthetic approach. Nat Chem 10:568-572 |
| Rupnik, Kresimir; Lee, Chi Chung; Hu, Yilin et al. (2018) A VTVH MCD and EPR Spectroscopic Study of the Maturation of the ""Second"" Nitrogenase P-Cluster. Inorg Chem 57:4719-4725 |
| Sickerman, Nathaniel S; Rettberg, Lee A; Lee, Chi Chung et al. (2017) Cluster assembly in nitrogenase. Essays Biochem 61:271-279 |
| Fay, Aaron W; Blank, Michael A; Rebelein, Johannes G et al. (2016) Assembly scaffold NifEN: A structural and functional homolog of the nitrogenase catalytic component. Proc Natl Acad Sci U S A 113:9504-8 |
| Hu, Yilin; Ribbe, Markus W (2016) Maturation of nitrogenase cofactor-the role of a class E radical SAM methyltransferase NifB. Curr Opin Chem Biol 31:188-94 |
| Lee, Chi Chung; Sickerman, Nathaniel S; Hu, Yilin et al. (2016) YedY: A Mononuclear Molybdenum Enzyme with a Redox-Active Ligand? Chembiochem 17:453-5 |
| Tanifuji, Kazuki; Lee, Chi Chung; Ohki, Yasuhiro et al. (2015) Combining a Nitrogenase Scaffold and a Synthetic Compound into an Artificial Enzyme. Angew Chem Int Ed Engl 54:14022-5 |
| Lee, Chi Chung; Hu, Yilin; Ribbe, Markus W (2015) Insights into hydrocarbon formation by nitrogenase cofactor homologs. MBio 6: |
| Ribbe, Markus W (2015) Insights into the Mechanism of Carbon Monoxide Dehydrogenase at Atomic Resolution. Angew Chem Int Ed Engl 54:8337-9 |
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