Evolution of electrochemically induced stress and its effect on the lithium-storage performance of graphite electrode

The electrochemically induced stress is a key factor that affects the lithium-storage performance of electrode materials.In this study,the origin and evolution of the electrochemically induced stress of the graphite electrode were investigated by in situ experiments and simulations.An in situ optical experiment was performed to observe the electrode color to analyze the concentration and diffusion process of lithium ions inside the graphite electrode.An electrochemical-mechanical coupling model under the same experimental conditions was developed and verified by the experimental lithium concentration,and characterization of the spatiotemporal evolution of the potential,lithium concentration,and stress during the diffusion process was realized.The results showed that lithium intercalation leads to compressive stress,which presents a gradient distribution along the Li+diffusion path,and it exhibits a“piecewise”nonlinear growth trend with increasing lithiation time.In addition,as the potential decreases,the stress increases from slow to fast relative to the lithium-concentration increase,showing the characteristic of stages.The influence of stress on the lithium-storage performance is discussed using the local lithium-intercalation rate and phase-interface migration speed as the key parameters.The lithiation mechanism was analyzed from the perspective of the energy,and it was found that the two factors cause the slow diffusion in the late stage of lithiation,thus affecting the actual lithium-storage performance.This study will enhance the understanding of the electro-chemo-mechanical coupling mechanism and provide guidance for enhancing stress-regulated battery performance.

Insights into Formation and Li-Storage Mechanisms of Hierarchical Accordion-Shape Orthorhombic CuNb_(2)O_(6) toward Lithium-Ion Capacitors as an Anode-Active Material

The orthorhombic CuNb_(2)O_(6)(O-CNO)is established as a competitive anode for lithium-ion capacitors(LICs)owing to its attractive compositional/structural merits.However,the high-temperature synthesis(>900℃)and controversial charge-storage mechanism always limit its applications.Herein,we develop a low-temperature strategy to fabricate a nano-blocks-constructed hierarchical accordional O-CNO framework by employing multilayered Nb_(2)CT_(x)as the niobium source.The intrinsic stress-induced formation/transformation mechanism of the monoclinic CuNb_(2)O_(6)to O-CNO is tentatively put forward.Furthermore,the integrated phase conversion and solid solution lithium-storage mechanism is reasonably unveiled with comprehensive in(ex)situ characterizations.Thanks to its unique structural merits and lithium-storage process,the resulted O-CNO anode is endowed with a large capacity of 150.3 mAh g^(-1)at 2.0 A g^(-1),along with long-duration cycling behaviors.Furthermore,the constructed O-CNO-based LICs exhibit a high energy(138.9 Wh kg^(-1))and power(4.0 kW kg^(-1))densities with a modest cycling stability(15.8%capacity degradation after 3000 consecutive cycles).More meaningfully,the in-depth insights into the formation and charge-storage process here can promote the extensive development of binary metal Nb-based oxides for advanced LICs.