Dependence of Initial Capacity Irreversibility on Oxygen Framework Chemistry in Li-Rich Layered Cathode Oxides

The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origin of specific active Li sites during discharge process.In this study,focusing on Ah-level pouch cells for reliability,an ultrahigh initial Coulombic efficiency(96.1%)is achieved in an archetypical Li-rich layered oxide material.Combining the structure and electrochemistry analysis,we demonstrate that the achievement of high-capacity reversibility is a kinetic effect,primarily related to the sluggish Li mobility during oxygen reduction.Activating oxygen reduction through small density would induce the oxygen framework contraction,which,according to Pauli repulsion,imposes a great repulsive force to hinder the transport of tetrahedral Li.The tetrahedral Li storage upon deep oxygen reduction is experimentally visualized and,more importantly,contributes to 6%Coulombic efficiency enhancement as well as 10%energy density improvement for pouch cells,which shows great potentials breaking through the capacity and energy limitation imposed by intercalation chemistry.

Practical evaluation of prelithiation strategies for next-generation lithium-ion batteries

With the increasing market demand for high-performance lithium-ion batteries with high-capacity electrode materials,reducing the irreversible capacity loss in the initial cycle and compensating for the active lithium loss during the cycling process are critical challenges.In recent years,various prelithiation strategies have been developed to overcome these issues.Since these approaches are carried out under a wide range of conditions,it is essential to evaluate their suitability for large-scale commercial applications.In this review,these strategies are categorized based on different battery assembling stages that they are implemented in,including active material synthesis,the slurry mixing process,electrode pretreatment,and battery fabrication.Furthermore,their advantages and disadvantages in commercial production are discussed from the perspective of thermodynamics and kinetics.This review aims to provide guidance for the future development of prelithiation strategies toward commercialization,which will potentially promote the practical application of next-generation high-energy-density lithium-ion batteries.

A high-durability aqueous Cu-S battery assisted by pre-copper electrochemistry

Although research interest in aqueous metal-sulfur batteries(AMSs)has surged due to their intrinsic low cost and high capacity,the practical application of AMSs remains a considerable challenge because of the restrictive cycling stability.To circumvent this issue,we propose an innovative and simple pre-copper strategy to realize a high-durability aqueous Cu-S battery.The precopper strategy can effectively promote a stable metal dissolution/deposition,compensate for charge carriers,and facilitate reaction kinetics during the subsequent process.As a result,the aqueous Cu-S battery when coupled with S-decorated porous Ti_(3)C_(2)(S-d-Ti_(3)C_(2))exhibits excellent electrochemical performance,delivering a highly reversible capacity of 1805.4 mAh·g^(-1)in the initial cycle at 0.8 A·g^(-1),impressive cycling stability with 90.2%capacity retention over 800 cycles,and ultralow polarization~0.08 V even at a high current density of 3.1 A·g^(-1).The findings obtained in this work could pave the way for the design of highperformance sulfur-based aqueous batteries,which fill the vacancy of the necessary metal anode,delivering merits in both cost and cycle life.

Recent advances and perspectives on prelithiation strategies for lithium-ion capacitors

Lithium-ion capacitors(LICs),consisting of a capacitor-type material and a battery-type material together with organic electrolytes,are the state-of-the-art electrochemical energy storage devices compared with supercapacitors and batteries.Owing to their unique characteristics,LICs received a lot of attentions,and great progresses have been achieved,especially in the exploration of cathode and anode materials.Prelithiation techniques are regarded as indispensable procedures for LICs systems,which can compensate for the initial irreversible capacity loss,increase the Li^(+)concentration in the electrolyte,raise the working voltage and resolve the safety and cycle stability issues;however,its research progress is slow,and there is not enough attention until now.In this overview,we look into the ongoing processes on the recent development of prelithiation technologies,especially in organic electrolyte consumption-type LICs.In particular,some prelithiation strategies for LICs are summarized and discussed in detail,including the ex situ electrochemical method,in situ electrochemical method,and cathode prelithiation additives method.Moreover,we propose some unresolved challenges and prospects for prelithiation technologies from the basic research ideas and future key research directions.This work aims to bring up new insights to reassess the significance of premetallation strategies for advanced hybrid-ion capacitors based on the currently proposed prelithiation strategies.