Nickel-rich (Ni-rich) cathode materials, LiNiCoMnO (NCM, x ≥ 0.9, x + y + z = 1) hold great promise for developing high energy density lithium ion batteries especially for vehicle electrification. However, the practical application of Ni-rich cathode materials is still suffered from fast structural and interfacial degradation, and the resulted capacity decay. In this study, a diazacyclo type electrolyte additive, 2-fluoropyrazine (2-FP), was explored for the first time to boost the interfacial stabilization of single crystal LiNiCoMnO (NCM90) cathode. The capacity retention of the NCM90 is evidently promoted from 72.3% to 82.1% after 200 cycles at 1C (180 mA g) when adding 0.2% 2-FP into the electrolyte. The improvement of the electrochemical performance is ascribed to the generation of a compact and homogeneous cathode electrolyte interphase (CEI) film through ring-opening electrochemical polymerization of 2-FP upon the NCM90 electrode particles. This enhanced CEI layer benefits the suppression of the decomposition of LiPF electrolyte and the dissolution of the transition metals (Co and Mn), thus preventing the detrimental side reactions between the NCM90 electrode and the electrolyte.
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http://dx.doi.org/10.1016/j.jcis.2022.03.089 | DOI Listing |
Org Lett
January 2025
Max-Planck-Institute for Chemical Energy Conversion, Stiftstraße 34-36, 45470 Mülheim an der Ruhr, Germany.
An electrochemical one-pot synthesis of enaminyl sulfonate esters was established, featuring a quasidivided cell under constant current conditions. The multicomponent reaction utilizes simple and readily available alkylamines and an easy-to-use stock solution of SO and alcohols. Omission of additional supporting electrolyte through in-situ-generated monoalkylsulfite facilitates the downstream processing.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Department of Applied Chemistry, Chuo University, Tokyo 112-8551, Japan.
We employed machine learning (ML) techniques combined with potential-dependent photoelectrochemical impedance spectroscopy (pot-PEIS) to gain deeper insights into the charge transport mechanisms of hematite (α-FeO) photoanodes. By the Shapley Additive exPlanations (SHAP) analysis from the ML model constructed from a small data set (dozens of samples) of electrical parameters obtained from pot-PEIS and the PEC performance, we identified the dominant factors influencing the electron transport to the back contact in the bulk and hole transfer to a solution at the hematite/electrolyte interface. The results revealed that shallow defect states significantly enhance electron transport, while deep defect states impede it, and also one of the surface states enhances the hole transfer to the electrolyte solution.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
School of Material Science and Engineering, Jiangsu Collaborative Innovation Center for Photovoltaic Science and Engineering, Jiangsu Province Cultivation Base for State Key Laboratory of Photovoltaic Science and Technology, Changzhou University, Changzhou 213164, China.
Lithium (Li) metal's extremely high specific energy and low potential make it critical for high-performance batteries. However, uncontrolled dendrite growth and an unstable solid-electrolyte interphase (SEI) during repeated cycling still seriously hinder its practical application in Li metal batteries. Herein, we demonstrate a facile and effective approach to fabricate a flexible and robust hybrid SEI layer using two kinds of organo-polysulfides with different sulfur chain lengths [bis(3-(triethoxysilyl)propyl)disulfide (Si-O-2S) and bis(3-(triethoxysilyl)propyl)tetrasulfide (Si-O-4S)] as the additives in the electrolyte.
View Article and Find Full Text PDFChem Sci
January 2025
State Key Laboratory of Powder Metallurgy, Central South University Changsha 410083 P. R. China
In overcoming the barrier of rapid Li transfer in lithium-ion batteries at extreme temperatures, the desolvation process and interfacial charge transport play critical roles. However, tuning the solvation structure and designing a kinetically stable electrode-electrolyte interface to achieve high-rate charging and discharging remain a challenge. Here, a lithium nonafluoro-1-butanesulfonate (NFSALi) additive is introduced to optimize stability and the robust solid electrolyte interface film (SEI), realizing a rapid Li transfer process and the structural integrity of electrode materials.
View Article and Find Full Text PDFACS Phys Chem Au
January 2025
Department of Fibre and Polymer Technology, Division of Coating Technology, KTH Royal Institute of Technology, SE-100 44 Stockholm, Sweden.
In an effort to improve safety and cycling stability of liquid electrolytes, the use of dicarbonates has been explored. In this study, four dicarbonate structures with varying end groups and spacers are investigated. The effect of these structural differences on the physical and ion transport properties is elucidated, showing that the end group has a significant influence on ion transport.
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