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Electron transfer in polysaccharide monooxygenase catalysis.
Proc Natl Acad Sci U S A
January 2025
California Institute for Quantitative Biosciences, University of California, Berkeley, CA 94720.
Polysaccharide monooxygenase (PMO) catalysis involves the chemically difficult hydroxylation of unactivated C-H bonds in carbohydrates. The reaction requires reducing equivalents and will utilize either oxygen or hydrogen peroxide as a cosubstrate. Two key mechanistic questions are addressed here: 1) How does the enzyme regulate the timely and tightly controlled electron delivery to the mononuclear copper active site, especially when bound substrate occludes the active site? and 2) How does this electron delivery differ when utilizing oxygen or hydrogen peroxide as a cosubstrate? Using a computational approach, potential paths of electron transfer (ET) to the active site copper ion were identified in a representative AA9 family PMO from (PMO9E).
View Article and Find Full Text PDFMicrobial-induced Synthesis of nano NiFe LDH for High-efficiency Oxygen Evolution.
Chemistry
January 2025
Wuhan University of Technology - Mafangshan Campus: Wuhan University of Technology, School of Material Science and Engineeringl, CHINA.
NiFe layered double hydroxide (LDH) currently are the most efficient catalysts for the oxygen evolution reaction (OER) in alkaline environments. However, the development of high-performance low cost OER electrocatalysts using straightforward strategies remains a significant challenge. In this study, we describe an innovative microbial mineralization-based method for in situ-induced preparation of NiFe LDH nanosheets loaded on nickel foam and demonstrate that this material serves as an efficient oxygen evolution electrocatalyst.
View Article and Find Full Text PDFMechanistic Understanding of the pH-Dependent Oxygen Reduction Reaction on the Fe-N-C Surface: Linking Surface Charge to Adsorbed Oxygen-Containing Species.
ACS Appl Mater Interfaces
January 2025
Center of Nanomaterials for Renewable Energy (CNRE), State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China.
The Fe-N-C catalyst, featuring a single-atom Fe-N configuration, is regarded as one of the most promising catalytic materials for the oxygen reduction reaction (ORR). However, the significant activity difference under acidic and alkaline conditions of Fe-N-C remains a long-standing puzzle. In this work, using extensive ab initio molecular dynamics (AIMD) simulations, we revealed that pH conditions influence ORR activity by tuning the surface charge density of the Fe-N-C surface, rather than through the direct involvement of HO or OH ions.
View Article and Find Full Text PDFCatalysis of a LiF-rich SEI by aromatic structure modified porous polyamine for stable all-solid-state lithium metal batteries.
Chem Sci
January 2025
School of Materials Science and Engineering, Xiangtan University Xiangtan 411105 China
Poly(ethylene oxide) (PEO)-based solid-state polymer electrolyte (SPE) is a promising candidate for the next generation of safer lithium-metal batteries. However, the serious side reaction between PEO and lithium metal and the uneven deposition of lithium ions lead to the growth of lithium dendrites and the rapid decline of battery cycle life. Building a LiF-rich solid electrolyte interface (SEI) layer is considered to be an effective means to solve the above problems.
View Article and Find Full Text PDFStepwise Structural Relaxation in Battery Active Materials.
ACS Mater Lett
January 2025
Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, PO Box 1033, Blindern 0315 Norway.
Whenever the cycling of Li-ion batteries is stopped, the electrode materials undergo a relaxation process, but the structural changes that occur during relaxation are not well-understood. We have used operando synchrotron X-ray diffraction with a time resolution of 1.24 s to observe the structural changes that occur when the lithiation of graphite and LiFePO electrodes are interrupted.
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