Low-Frequency Phonon Dispersion Relation Enabling Stable Cathode from Spent Lithium-Ion Batteries.

Direct recycling technology can effectively solve the environmental pollution and resource waste problems caused by spent lithium-ion batteries. However, the repaired LiNiCoMnO (NCM) black mass by direct recycling technology shows an unsatisfactory cycle life, which is attributed to the formation of spinel/rock salt phases and rotational stacking faults caused by the in-plane and out-of-plane migration of transition metal (TM) atoms during charge/discharge. Herein, local lattice stress is introduced into the regenerated cathode during repair.

Optimizing s-p Orbital Overlap between Sodium Polysulfides and Single-Atom Indium Catalyst for Efficient Sulfur Redox Reaction.

P-block metal carbon-supported single-atom catalysts (C-SACs) have emerged as a promising candidate for high-performance room-temperature sodium-sulfur (RT Na-S) batteries, due to their high atom utilization and unique electronic structure. However, the ambiguous electronic-level understanding of Na-dominant s-p hybridization between sodium polysulfides (NaPSs) and p-block C-SACs limits the precise control of coordination environment tuning and electro-catalytic activity manipulation. Here, s-p orbital overlap degree (OOD) between the s orbitals of Na in NaPSs and the p orbitals of p-block C-SACs is proposed as a descriptor for sulfur reduction reaction (SRR) and sulfur oxidation reaction (SOR).

High-Capacity and Long-Life Aqueous Zn-SPAN Batteries with Tandem Catalysis.

Aqueous zinc-sulfur batteries are a high-capacity and cost-effective energy storage technology. However, the performance is plagued by the dissolution of intermediate polysulfides formed during conversion. Here, this issue is addressed by developing aqueous rechargeable Zn-sulfurized polyacrylonitrile (SPAN) batteries using tandem catalytic systems, containing water and tetraglyme (G4) with iodine (I) additives.

Dynamic Imine Chemistry Enables Paintable Biogel Electrolytes to Shield On-Body Zinc-Ion Batteries from Interfacial Interference.

On-body batteries with hydrogel electrolytes are a pivotal enabling technology to drive bioelectronics for healthcare and sports, yet they are prone to failure due to dynamic interfacial interference, accompanied by e-waste production. Here, dynamic imine chemistry is proposed to design on-electrode paintable biogel electrolytes that feature temperature-controlled reversible phase transition (gelling within 1.5 min) and ultrafast self-healing capability (6 s), establishing a dynamically self-adaptive interface on cyclically deforming electrodes for shielding on-body Zn-ion batteries from interfacial interference.

Large scalable nickel phosphide/nickel@carbon cloth-based flexible composite electrodes for symmetric supercapacitors.

A flexible NiP/Ni@CC composite electrode with remarkable mechanical robustness is developed by a scalable and facile synthetic approach. The as-constructed symmetric supercapacitor demonstrates impressive energy density (51.1 W h kg) at a high power density (3500 W kg) along with excellent cycling stability.

Generative learning assisted state-of-health estimation for sustainable battery recycling with random retirement conditions.

Rapid and accurate state of health (SOH) estimation of retired batteries is a crucial pretreatment for reuse and recycling. However, data-driven methods require exhaustive data curation under random SOH and state of charge (SOC) retirement conditions. Here, we show that the generative learning-assisted SOH estimation is promising in alleviating data scarcity and heterogeneity challenges, validated through a pulse injection dataset of 2700 retired lithium-ion battery samples, covering 3 cathode material types, 3 physical formats, 4 capacity designs, and 4 historical usages with 10 SOC levels.

Exclusive Generation of Single-Atom Sulfur for Ultrahigh Quality Monolayer MoS Growth.

Preparation of high-quality two-dimensional (2D) transition metal dichalcogenides (TMDCs) is the precondition for realizing their applications. However, the synthesized 2D TMDCs (e.g.

Direct Regeneration of Industrial LiFePO Black Mass Through A Glycerol-Enabled Granule Reconstruction Strategy.

With the increasing sales of electric vehicles, lots of spent lithium-ion batteries (LIBs) assembled with LiFePO (LFP) cathodes will retire in the next few years, posing a significant challenge for their effective and environmentally-friendly recycling. The main reason why spent LFP cathodes fail to re-utilize lies in the lattice defects caused by lithium loss and structural defects resulting from stress accumulation. In this work, we propose an in situ granule reconstruction strategy to directly regenerate spent LFP black mass (S-BM) using glycerol in industry settings.

Machine learning-based design of electrocatalytic materials towards high-energy lithium||sulfur batteries development.

The practical development of Li | |S batteries is hindered by the slow kinetics of polysulfides conversion reactions during cycling. To circumvent this limitation, researchers suggested the use of transition metal-based electrocatalytic materials in the sulfur-based positive electrode. However, the atomic-level interactions among multiple electrocatalytic sites are not fully understood.

Recent Advances in High-Entropy Layered Oxide Cathode Materials for Alkali Metal-Ion Batteries.

Since the electrochemical de/intercalation behavior is first detected in 1980, layered oxides have become the most promising cathode material for alkali metal-ion batteries (Li/Na/K; AMIBs) owing to their facile synthesis and excellent theoretical capacities. However, the inherent drawbacks of unstable structural evolution and sluggish diffusion kinetics deteriorate their electrochemical performance, limiting further large-scale applications. To solve these issues, the novel and promising strategy of high entropy has been widely applied to layered oxide cathodes for AMIBs in recent years.

Targeted Defect Repair and Multi-functional Interface Construction for the Direct Regeneration of Spent LiFePO Cathodes.

Due to the low economic benefits and environmental pollution of traditional recycling methods, the disposal of spent LiFePO (SLFP) presents a significant challenge. The capacity fade of SLFP cathode is primarily caused by lithium loss and formation of a Fe (III) phase. Herein, a synergistic repair effect is proposed to achieve defect repair and multi-functional interface construction for the direct regeneration of SLFP.

Surface Catalytic Repair for the Efficient Regeneration of Spent Layered Oxide Cathodes.

Direct recycling is considered to be the next-generation recycling technology for spent lithium-ion batteries due to its potential economic benefits and environmental friendliness. For the spent layered oxide cathode materials, an irreversible phase transition to a rock-salt structure near the particle surface impedes the reintercalation of lithium ions, thereby hindering the lithium compensation process from fully restoring composition defects and repairing failed structures. We introduced a transition-metal hydroxide precursor, utilizing its surface catalytic activity produced during annealing to convert the rock-salt structure into a layered structure that provides fast migration pathways for lithium ions.

Routes to Bidirectional Cathodes for Reversible Aprotic Alkali Metal-CO Batteries.

Aprotic alkali metal-CO batteries (AAMCBs) have garnered significant interest owing to fixing CO and providing large energy storage capacity. The practical implementation of AAMCBs is constrained by the sluggish kinetics of the CO reduction reaction (CORR) and the CO evolution reaction (COER). Because the COER and CORR take place on the cathode, which connects the internal catalyst with the external environment.

Bimetal Fluorides with Adjustable Vacancy Concentration Reinforcing Ion Transport in Poly(ethylene oxide) Electrolyte.

The poor ambient ionic transport properties of poly(ethylene oxide) (PEO)-based SPEs can be greatly improved through filler introduction. Metal fluorides are effective in promoting the dissociation of lithium salts via the establishment of the Li-F bond. However, too strong Li-F interaction would impair the fast migration of lithium ions.

MXene Triggered Free Radical Polymerization in Minutes Toward All-Printed Zn-Ion Hybrid Capacitors and Beyond.

Additive manufacturing of (quasi-) solid-state (QSS) electrochemical energy storage devices (EES) highlights the significance of gel polymer electrolytes (GPEs) design. Creating well-bonded electrode-GPEs interfaces in the electrode percolative network via printing leads to large-scale production of customized EES with boosted electrochemical performance but has proven to be quite challenging. Herein, we report on a versatile, universal and scalable approach to engineer a controllable, seamless electrode-GPEs interface via free radical polymerization (FRP) triggered by MXene at room temperature.

Pathway decisions for reuse and recycling of retired lithium-ion batteries considering economic and environmental functions.

Reuse and recycling of retired electric vehicle (EV) batteries offer a sustainable waste management approach but face decision-making challenges. Based on the process-based life cycle assessment method, we present a strategy to optimize pathways of retired battery treatments economically and environmentally. The strategy is applied to various reuse scenarios with capacity configurations, including energy storage systems, communication base stations, and low-speed vehicles.

Activated Co in Thiospinel Boosting LiCO Decomposition in Li-CO Batteries.

Catalytic reactions mainly depend on the adsorption properties of reactants on the catalyst, which provides a perspective for the design of reversible lithium-carbon dioxide (Li-CO) batteries including CO reduction (CORR) and CO evolution (COER) reactions. However, due to the complex reaction process, the relationship between the adsorption configuration and CORR/COER catalytic activity is still unclear in Li─CO batteries. Herein, taking CoS as a model system, nickel (Ni substitution in the tetrahedral site to activate cobalt (Co) atom for forming multiatom catalytic domains in NiCoS is utilized.

High-voltage electrosynthesis of organic-inorganic hybrid with ultrahigh fluorine content toward fast Li-ion transport.

Hybrid materials with a rational organic-inorganic configuration can offer multifunctionality and superior properties. This principle is crucial but challenging to be applied in designing the solid electrolyte interphase (SEI) on lithium metal anodes (LMAs), as it substantially affects Li transport from the electrolyte to the anode. Here, an artificial SEI with an ultrahigh fluorine content (as high as 70.

Steering the Orbital Hybridization to Boost the Redox Kinetics for Efficient Li-CO Batteries.

The sluggish CO reduction and evolution reaction kinetics are thorny problems for developing high-performance Li-CO batteries. For the complicated multiphase reactions and multielectron transfer processes in Li-CO batteries, exploring efficient cathode catalysts and understanding the interplay between structure and activity are crucial to couple with these pendent challenges. In this work, we applied the CoS as a model catalyst and adjusted its electronic structure by introducing sulfur vacancies to optimize the d-band and p-band centers, which steer the orbital hybridization and boost the redox kinetics between Li and CO, thus improving the discharge platform of Li-CO batteries and altering the deposition behavior of discharge products.