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Morphology-Transport Coupling and Dissipative Structures in PEO-PS+LiTFSI Electrolytes In-Operando Conditions.
ACS Appl Mater Interfaces
January 2025
Institute for Theoretical Physics, Georg-August University of Göttingen, 37077 Göttingen, Germany.
A Single-Chain-in-Mean-Field (SCMF) algorithm was introduced to study block copolymer electrolytes in nonequilibrium conditions. This method self-consistently combines a particle-based description of the polymer with a generalized diffusion equation for the ionic fluxes, thus exploiting the time scale separation between fast ion motion and the slow polymer relaxation and self-assembly. We apply this computational method to study ion fluxes in electrochemical cells containing poly(ethylene oxide)-polystyrene (PEO-PS) block copolymers with added lithium salt.
View Article and Find Full Text PDFRegulating the Thermodynamic Uniformity and Kinetic Diffusion of Zinc Anodes for Deep Cycling of Ah-Level Aqueous Zinc-Metal Batteries.
ACS Nano
January 2025
Power Battery & Systems Research Center, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Zn metal anodes in mildly acidic electrolytes usually suffer from a series of problems, including parasitic dendrite growth and severe side reactions, significantly limiting the Zn utilization efficiency and cycling life. A deep understanding of the Zn stripping/plating process is essential to obtain high-efficiency and long-life Zn metal anodes. Here, the factors affecting the Zn stripping/plating process are revealed, suggesting that thermodynamic uniformity in bulk structures promotes an orderly Zn stripping process, and a fast kinetic diffusion rate on the Zn surface facilitates uniform Zn deposition.
View Article and Find Full Text PDFNumerical analysis of sodium diffusion in aluminum electrolysis cathode carbon blocks based on a microstructure multi-factor corrected model.
PLoS One
January 2025
The Key Laboratory of Cyber-Physical Power System of Yunnan Universities, Yunnan Minzu University, Kunming, Yunnan Province, China.
Current researches on sodium penetration in electrolytic aluminum cathode carbon blocks primarily measure cathode expansion curves, showing mostly macroscopic characteristics. However, the microscopic structure is often underexplored. As a porous medium, the diffusion performance of cathode carbon blocks is closely tied to their internal pore structure.
View Article and Find Full Text PDFElectrocatalysis: From Planar Surfaces to Nanostructured Interfaces.
Chem Rev
January 2025
Department of Chemical & Biomolecular Engineering, University of California, Irvine, California 92697, United States.
The reactions critical for the energy transition center on the chemistry of hydrogen, oxygen, carbon, and the heterogeneous catalyst surfaces that make up electrochemical energy conversion systems. Together, the surface-adsorbate interactions constitute the electrochemical interphase and define reaction kinetics of many clean energy technologies. Practical devices introduce high levels of complexity where surface roughness, structure, composition, and morphology combine with electrolyte, pH, diffusion, and system level limitations to challenge our ability to deconvolute underlying phenomena.
View Article and Find Full Text PDFNon-monotonic Variation of Potential-dependent Surface Diffusion at Electrochemical Interfaces in the Presence of Coadsorbates.
Angew Chem Int Ed Engl
January 2025
University of Kiel, Physics, Olshausenstr. 40, 24098, Kiel, GERMANY.
The influence of coadsorbed ions on adsorbate diffusion, an inherent effect at solid-liquid interfaces, was studied for adsorbed sulfur on Ag(100) electrodes in the presence of bromide or iodide. Quantitative in situ high-speed scanning tunnelling microscopy (video-STM) measurements were performed both in the potential regime of the c(2×2) halide adlayer at its saturation coverage and in the regime of a disordered adlayer where the halide coverage increases with potential. These studies reveal a surprising non-monotonic potential dependence of Sad diffusion with an initial increase with halide coverage, followed by a decrease upon halide adlayer ordering into the c(2×2) structure.
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