An asymmetric sulfur ylide reaction was employed to prepare an epoxide intermediate in a convergent manner. This epoxide was efficiently transformed into D-erythro-sphingosine.
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Low-valence platinum single atoms in sulfur-containing covalent organic frameworks for photocatalytic hydrogen evolution.
Nat Commun
December 2024
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, China.
This study focuses on optimizing catalytic activity in photocatalytic hydrogen evolution reaction by precisely designing and modulating the electronic structure of metal single atoms. The catalyst, denoted as PtSA@S-TFPT, integrates low-valence platinum single atoms into sulfur-containing covalent organic frameworks. The robust asymmetric four-coordination between sulfur and platinum within the framework enables a high platinum loading of 12.
View Article and Find Full Text PDFStructural evolution of nitrogenase states under alkaline turnover.
Nat Commun
December 2024
Division of Chemistry and Chemical Engineering 147-75 California Institute of Technology, Pasadena, CA, USA.
Biological nitrogen fixation, performed by the enzyme nitrogenase, supplies nearly 50% of the bioavailable nitrogen pool on Earth, yet the structural nature of the enzyme intermediates involved in this cycle remains ambiguous. Here we present four high resolution cryoEM structures of the nitrogenase MoFe-protein, sampled along a time course of alkaline reaction mixtures under an acetylene atmosphere. This series of structures reveals a sequence of salient changes including perturbations to the inorganic framework of the FeMo-cofactor; depletion of the homocitrate moiety; diminished density around the S2B belt sulfur of the FeMo-cofactor; rearrangements of cluster-adjacent side chains; and the asymmetric displacement of the FeMo-cofactor.
View Article and Find Full Text PDFAsymmetric Polarization Modulation of d-p Hybridization-Enhanced Bidirectional Sulfur Redox Kinetics with Heteronuclear Dual-Atom Catalysts.
ACS Nano
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Department of Materials Science and Engineering, National University of Singapore, Singapore 117574, Republic of Singapore.
Lithium sulfur batteries (LiSBs) represent a highly promising avenue for future energy storage systems, offering high energy density and eco-friendliness. However, the sluggish kinetics of the sulfur redox reaction (SRR) poses a significant challenge to their widespread applications. To tackle this challenge, we have developed an efficient heteronuclear dual-atom catalyst (hetero-DAC) that leverages surface charge polarization to enhance the asymmetric adsorption of sulfur intermediates.
View Article and Find Full Text PDFAnisotropic Etching of Monolayer MoS Flakes for Zigzag Edges in Chemical Vapor Deposition.
ACS Appl Mater Interfaces
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National Laboratory of Solid State Microstructures, School of Physics, Collaborative Innovation Center of Advanced Microstructures, and Jiangsu Physical Science Research Center, Nanjing University, Nanjing 210093, China.
The edge of two-dimensional (2D) flakes of transition metal dichalcogenide (TMD) profoundly influences their optical, electronic, catalytic, and magnetic properties due to the asymmetric atomic configurations on the edge. As a reverse process of growth, the etching of monolayer MoS flakes can be modulated by tuning the sulfur stoichiometric ratio in chemical vapor deposition. Here, we report studies of the high-density formation of etched pores with defined orientations on MoS flakes.
View Article and Find Full Text PDFUnraveling energetics and states of adsorbing oxygen species with MoS for modulated work function.
Nanoscale Horiz
November 2024
Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Taipa, Macau, China.
MoS and related transition metal dichalcogenides (TMDs) have recently been reported as having extensive applications in nanoelectronics and catalysis because of their unique physical and chemical properties. However, one practical challenge for MoS-based applications arises from the easiness of oxygen contamination, which is likely to degrade performance. To this end, understanding the states and related energetics of adsorbed oxygen is critical.
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