Article
Chemistry, Multidisciplinary
Golam Moula, Ayaka Nagasaki, Tsuyoshi Matsumoto, Matthias E. Miehlich, Karsten Meyer, Roger E. Cramer, Kazuyuki Tatsumi
Summary: The construction of synthetic models of the nitrogenase P-N-cluster has been a long-standing challenge, and the closest mimic constructed to date is the optimal nitrogenase P-N-cluster model represented by cluster 2. The model has been characterized by X-ray crystallography and relevant physico-chemical methods, revealing its magnetic and Mossbauer spectrum properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Multidisciplinary
Yilin Hu, Chi Chung Lee, Mario Grosch, Joseph B. Solomon, Wolfgang Weigand, Markus W. Ribbe
Summary: The Fischer-Tropsch (FT) process is used to convert a mixture of CO and H2 into liquid hydrocarbons for synthetic fuel production. However, enzymatic FT-type reactions, catalyzed by nitrogenase enzymes, metalloclusters and synthetic mimics, can also convert CO, CO2, and CN- into hydrocarbons under ambient conditions using H+ and e- as reducing equivalents. This review provides an overview of nitrogenase enzymes and metalloclusters, discusses the activities of nitrogenase-derived FT systems, and explores the mechanistic, evolutionary, and biotechnological implications of enzymatic FT reactions.
Article
Chemistry, Multidisciplinary
Valerie Waser, Manjistha Mukherjee, Nico V. Igareta, Ryo V. Tachibana, Thomas R. R. Ward
Summary: Researchers designed and assembled an artificial [Fe4S4]-containing Fischer-Tropsch catalyst using biotin-streptavidin technology. They synthesized a stable bis-biotinylated [Fe4S4] cofactor and incorporated it in streptavidin. The effect of the protein environment on catalytic activity was investigated, and the catalyst exhibited up to 14 turnovers for the reduction of CO2 to hydrocarbons.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Alexandra C. Brown, Daniel L. M. Suess
Summary: Attempts to generate open coordination sites for N2 binding at synthetic Fe-S clusters often result in cluster oligomerization. However, recent studies have shown that oligomerization reactions can be prevented by using sterically protective supporting ligands in Mo-Fe-S clusters, enabling N2 complex formation. This strategy has now been extended to Fe-only Fe-S clusters. Evaluation: 7 out of 10.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Zhi-Yong Yang, Lance C. Seefeldt, Artavazd Badalyan, Brian M. Hoffman, Dennis R. Dean
Summary: A central feature of the current understanding of dinitrogen reduction by nitrogenase is the proposed coupling of ATP hydrolysis to electron transfer. Recent studies have shown that the Fe protein cluster can be further reduced to a super-reduced state. It has been suggested that this super-reduced state may change the existing model for nitrogenase energy utilization. However, it has been found that both oxidation states of the Fe protein still require hydrolysis of two ATP for each single-electron transfer.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Joseph B. Solomon, Mahtab F. Rasekh, Caleb J. Hiller, Chi Chung Lee, Kazuki Tanifuji, Markus W. Ribbe, Yilin Hu
Summary: The Fe proteins MaNifH and MaVnfH from Methanosarcina acetivorans exhibit different reactivities towards C1 substrates in the all-ferrous state, with MaVnfH showing weaker reactivity due to adopting the all-ferrous state at a more positive reduction potential. This suggests the possibility of MaVnfH accessing the all-ferrous state under physiological conditions, which has implications for the reaction mechanism of nitrogenase.
Article
Multidisciplinary Sciences
Liam Grunwald, Martin Clemancey, Daniel Klose, Lionel Dubois, Serge Gambarelli, Gunnar Jeschke, Michael Worle, Genevieve Blondin, Victor Mougel
Summary: A complete series of [Fe4S4](n) complexes spanning all redox states accessible by 1-electron transformations of the individual iron atoms has been successfully synthesized using a bulky arylthiolate ligand. The characterization results suggest a systematic correlation between the geometry of the Fe4S4 core and the oxidation state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Multidisciplinary
Hannah L. Rutledge, Mackenzie J. Field, Jonathan Rittle, Michael T. Green, F. Akif Tezcan
Summary: Nitrogenase catalyzes the reduction of dinitrogen to ammonia, with P-cluster and fiSer188 playing a protective role. The study reveals the importance of fiSer188 for the function and growth of nitrogenase.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Carlos Martin-Fernandez, Jeremy N. Harvey
Summary: The study discusses the relationship between errors in density functional theory and errors in self-consistent densities obtained from different density functional approximations, as well as how to measure and evaluate density sensitivity. Two widely applicable metrics for any density functional approximation are reported, along with how they can be used to classify chemical systems based on their sensitivity to small variations in density.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Review
Medicine, General & Internal
T. Rogier, C. Auvens, T. Thibault, S. Mouries-Martin, G. Muller, N. El Hssaini, A. Turcu, J. -f. Besancenot, P. Bielefeld, H. Devilliers
Summary: This study aimed to explore the use of colchicine in non-severe ocular inflammatory disease. The results of the study showed that colchicine was considered effective in some analyzable patients. Therefore, colchicine may be a treatment option for non-granulomatous anterior uveitis and non-severe recurrent scleritis.
REVUE DE MEDECINE INTERNE
(2022)