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351.
Yudhajeet Basak Dr. Jae-Hun Jeoung Dr. Lilith Domnik Prof. Dr. Holger Dobbek 《Angewandte Chemie (International ed. in English)》2023,62(32):e202305341
Ni,Fe-containing carbon monoxide dehydrogenases (CODHs) catalyze the reversible reduction of carbon dioxide to carbon monoxide. CODHs are found in anaerobic microorganisms and can rapidly lose their activity when exposed to air. What causes the loss of activity is unclear. In this study, we analyzed the time-dependent structural changes induced by the presence of air on the metal centers of CODH-II. We show that inactivation is a multistep process. In a reversible step, the open coordination site on the Ni ion is blocked by a Ni,Fe-bridging μ-sulfido or chlorido ligand. Blocking this open coordination site with a cyanide ligand stabilizes the cluster against O2-induced decomposition, indicating that O2 attacks at the Ni ion. In the subsequent irreversible phase, nickel is lost, the Fe ions rearrange and the sulfido ligands disappear. Our data are consistent with a reversible reductive reactivation mechanism to protect CODHs from transient over-oxidation. 相似文献
352.
For a -regular connected graph H the problem of determining the upper tail large deviation for the number of copies of H in , an Erdős-Rényi graph on n vertices with edge probability p, has generated significant interest. For and , where is the number of vertices in H, the upper tail large deviation event is believed to occur due to the presence of localized structures. In this regime the large deviation event that the number of copies of H in exceeds its expectation by a constant factor is predicted to hold at a speed , and the rate function is conjectured to be given by the solution of a mean-field variational problem. After a series of developments in recent years, covering progressively broader ranges of p, the upper tail large deviations for cliques of fixed size were proved by Harel, Mousset, and Samotij in the entire localized regime. This paper establishes the conjecture for all connected regular graphs in the whole localized regime. © 2021 Wiley Periodicals LLC. 相似文献
353.
Vijay Babu Pathi Arindam Manna Ravuri Srinath Supriyo Adhikary Prof. Dr. Biswadip Banerji 《European journal of organic chemistry》2023,26(28):e202300256
Regioselective synthesis of N-fused benzimidazo-indolo-isoquinoline heterocycles via Pd-catalyzed domino coupling reaction of 1-(1-methyl-1H-indol-2-yl)-1H-benzimidazoles and aryl halides was developed. This one pot methodology proceeded via a five-member carbopalladacycle intermediate and provided direct and facile route to access structurally complex polyheterocycles in moderate to good yields. These unique hybrid molecules resembled structural similarity with naturally isolated alkaloids. Notably, the present domino process occurred through activation of three C−H bonds and the simultaneous formation of two new C−C bonds in one-shot. These molecules exhibited strong solid and solution phase fluorescence and their emission spectra in both the medium are reported here. 相似文献