A structural model for the active site of phosphoesterases, enzymes that degrade organophosphate neurotoxins, has been synthesised. The ligand [2-((2-hydroxy-3-(((2-hydroxyethyl)(pyridin-2-ylmethyl)amino)methyl)-5-methylbenzyl)(pyridin-2-ylmethyl)amino)acetic acid] (H(3)L1) and two Zn(ii) complexes have been prepared and characterised as [Zn(2)(HL1)(CH(3)COO)](PF(6)).H(2)O and Li[Zn(2)(HL1)](4)(PO(4))(2)(PF(6))(3).(CH(3)OH). The ligand (H(3)L1) and complex [Zn(2)(HL1)(CH(3)COO)](PF(6)).H(2)O were characterised through (1)H NMR, (13)C NMR, mass spectroscopy and microanalysis. The X-ray crystal structure of Li[Zn(2)(HL1)](4)(PO(4))(2)(PF(6))(3).(CH(3)OH) revealed a tetramer of dinuclear complexes, bridged by two phosphate molecules and bifurcating acetic acid arms. Functional studies of the zinc complex with the substrate bis(4-nitrophenyl)phosphate (bNPP) determined the complex with HL1(2-) to be a competent catalyst with k(cat) = 1.26 +/- 0.06 x 10(-6) s(-1).
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http://dx.doi.org/10.1039/b806391e | DOI Listing |
ACS Appl Mater Interfaces
January 2025
The Institute for Advanced Studies, Wuhan University, Wuhan, Hubei 430072, People's Republic of China.
Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in the heterogeneous system and the limited recyclability in the homogeneous system significantly hinder the advancement of dehalogenative deuteration. In this study, we present a catalyst composed of copper single-atom sites anchored within an ordered mesoporous nitrogen-doped carbon matrix, synthesized via a mesopore confinement method.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2025
Instituto de Biología Molecular y Celular de Plantas, Consejo Superior de Investigaciones Científicas-Universitat Politècnica de València, Valencia 46022, Spain.
The SWItch/Sucrose Non-Fermenting (SWI/SNF) complexes are evolutionarily conserved, ATP-dependent chromatin remodelers crucial for multiple nuclear functions in eukaryotes. Recently, plant BCL-DOMAIN HOMOLOG (BDH) proteins were identified as shared subunits of all plant SWI/SNF complexes, significantly impacting chromatin accessibility and various developmental processes in Arabidopsis. In this study, we performed a comprehensive characterization of mutants, revealing the role of BDH in hypocotyl cell elongation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
East China University of Science and Technology, Key Laboratory for Advanced Materials and Institute of Fine Chemicals, 130 Meilong Road, 200237, Shanghai, CHINA.
Nanoconfinement at the interface of heterogeneous Fenton-like catalysts offers promising avenues for advancing oxidation processes in water purification. Herein, we introduce a template-free strategy for synthesizing nanoconfined catalysts from municipal sludge (S-NCCs), specifically engineered to optimize reactive oxygen species (ROS) generation and utilization for rapid pollutant degradation. Using selective hydrofluoric acid corrosion, we create an architecture that confines atomically dispersed Fe centers within a micro-mesoporous carbon matrix in situ.
View Article and Find Full Text PDFDoping strategies have been recognized as effective approaches for developing cost-effective and durable catalysts with enhanced reactivity and selectivity in the electrochemical synthesis of value-added compounds directly from CO. However, the reaction mechanism and the specific roles of heteroatom doping, such as N doping, in advancing the CO reduction reaction are still controversial due to the lack of precise control of catalyst surface microenvironments. In this study, we investigated the effects of N doping on the performances for electrochemically converting CO to CO over Ni@NCNT/graphene hybrid structured catalysts (Ni@NCNT/Gr).
View Article and Find Full Text PDFChem Sci
January 2025
Molecular Horizons and School of Chemistry and Molecular Bioscience, University of Wollongong Wollongong New South Wales 2522 Australia
Although electrostatic catalysis can enhance the kinetics and selectivity of reactions to produce greener synthetic processes, the highly directional nature of electrostatic interactions has limited widespread application. In this study, the influence of oriented electric fields (OEF) on radical addition and atom abstraction reactions are systematically explored with ion-trap mass spectrometry using structurally diverse distonic radical ions that maintain spatially separated charge and radical moieties. When installed on rigid molecular scaffolds, charged functional groups lock the magnitude and orientation of the internal electric field with respect to the radical site, creating an OEF which tunes the reactivity across the set of gas-phase carbon-centred radical reactions.
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