Electrochemical Performance Research Articles

Tuning Ce-doping La0.7Sr0.3Fe0.9Ni0.1O3-δ internal reforming catalyst to enhanced conversion efficiency and coking tolerance of solid oxide fuel cells fueled by oxygen-bearing low concentration coal mine methane

Solid oxide fuel cells (SOFCs) possess the potential to directly utilize abundant low concentration coal mine methane for power generation, which is crucial for energy conservation and reducing greenhouse gas emissions. Herein, Ce-doped La0.55Ce0.15Sr0.3Fe0.9Ni0.1O3-δ (LCSFN) perovskite is firstly employed as an anode internal reforming catalyst to enhance the electrochemical performance, stability, and resistance against carbon deposition in SOFCs. The results demonstrate that Ni-Fe alloy nanoparticles can be effectively precipitated from LCSFN under reducing atmosphere, thereby significantly promoting the partial oxidation reaction of methane while preventing direct contact between methane and Ni particles for the anode. The anode-supported single cells demonstrated exceptional electrochemical performance using a composite catalytic layer consisting of LCSFN-Ce0.9Gd0.1O2-δ (LCSFN-GDC). At 800℃, the utilization of both H2 and 16 %CH4-1 %O2-N2 resulted in the attainment of maximum power densities (MPD) measuring 881.66 mW·cm−2 and 824.69 mW·cm−2, respectively, with the recorded values for polarization resistance were 0.32 and 1.16 Ω·cm2. Additionally, the single cells equipped with LCSFN-GDC internal reforming catalytic exhibit remarkable resistance to carbon deposition, maintaining stable performance for a duration of 100 h using 16 %CH4-1 %O2-N2. These findings underscore the efficacy of methane catalysts in SOFCs, as it not only enhances power generation efficiency through using internal reforming catalyst but also ensures long-term stability by mitigating carbon-related issues.

Microstructure, electrochemical corrosion and corrosion mechanism of electroplated Ni–W alloy coating by DFT calculation

ABSTRACT A Ni–W alloy coating with a thickness of 5 μm was electroplated on N80 steel, and its electrochemical performance in a 3.5% NaCl solution was investigated. The atomic models of passive films and corrosion mechanism were analysed with the density functional theory calculation. The results show that the electroplated Ni–W alloy coating is composed of W atoms in the Ni lattice, and its surface roughness and particle size are 66.1 and 640.4 nm, respectively. The corrosion current density of Ni–W coating is lower than that of the substrate, indicating better corrosion resistance, while the corrosion potential is opposite, which is more passive than the substrate. The total impedance of Ni–W coating is higher than that of the substrate, which is attributed to the formation of NiO passive film during the corrosion process.

Adjusting Ion Diffusion Kinetics of Li Deposition Enabled by an Elastic Porous Melamine Sponge Host for Stable Lithium Metal Anodes.

Lithium (Li) dendritic growth and huge volume expansion seriously hamper Li-metal anode development. Herein, we design a lightweight 3D Li-ion-affinity host enabled by silver (Ag) nanoparticles fully decorating a porous melamine sponge (Ag@PMS) for dendrite-free and high-areal-capacity Li anodes. The compact Ag nanoparticles provide abundant preferred nucleation sites and give the host strong conductivity. Moreover, the high specific surface area and polar groups of the elastic, porous melamine sponge enhance the Li-ion diffusion kinetics, prompting homogeneity of Li deposition and stripping. As expected, the integrated 3D Ag@PMS-Li anode delivered a remarkable electrochemical performance, with a Coulombic efficiency (CE) of 97.14% after 450 cycles at 1 mA cm-2. The symmetric cell showed an ultralong lifespan of 3400 h at 1 mA cm-2 for 1 mAh cm-2. This study provides a facile and cost-effective strategy to design an advanced 3D framework for the preparation of a stable dendrite-free Li metal anode.

Suppressing Formation of Zn─Mn─O Phases by In Situ Ti Decoration of MnO2 for Long Lifespan MnO2-Zn Battery.

Mildly-acidic MnO2-Zn batteries are considered as a promising alternative for large-scale energy storage systems for their low toxicity, high safety, and low cost. Though, the degradation of MnO2 with cycling still hinders the further development of the batteries. In this study, it is observed that the decrease in available capacity of MnO2 with charge and discharge is accompanied by a structural transformation with the emergence of Zn─Mn─O phases. An electrodeposition test indicates that the Zn─Mn─O phase is formed from a co-precipitation of Zn and Mn during the charge process. Further, the structural change of MnO2 is suppressed and its cycle stability is improved with the addition of TiOSO4 as a facile electrolyte additive. As a result, under a current of 1200mA g-1, the MnO2 electrode still gives a capacity of 230 mAh g-1 for over 1500 cycles. Capacity retention is 75% after 10000 cycles under a current rate of 4800mA g-1. These findings provide fundamental insights on the degradation mechanism of MnO2 and a new strategy to improve the electrochemical performance of aqueous MnO2-Zn batteries.

Tribological and electrochemical behaviour study of porous TiNiCu alloys manufactured by the powder metallurgy process

ABSTRACT The experimental work aims to study the effect of the Copper (Cu) addition on the tribological and electrochemical behaviour of porous Ti50Ni50-x-Cux alloys. In the first step pure metal powders of titanium (Ti), nickel (Ni), and Cu were ball-milled during 8 h in a planetary ball mill, and then compacted under a 4 ton load to obtain pre-alloyed powders. The final step is sintering at 950°C for 7 h in a tubular furnace under a controlled atmosphere. X-ray diffraction measurements (XRD), scanning electron microscopy (SEM) analyses, microhardness measurements, friction tests and electrochemical were carried out to characterise the tribological and electrochemical performances of the elaborated specimens. DRX results reveal the formation of four major phases: TiNi, Ti2Ni, TiNi3 and TiNi0.8Cu0.2. Potentiodynamic polarisation tests show the positive effect of adding Cu on corrosion resistance, where the 6% Cu sample exhibits the best corrosion behaviour. Tribological results show a decrease in the coefficient of friction and wear rate with the addition of Cu, compared to the initial state, without Cu addition. The minimum coefficient of friction (0.585) was recorded for the 2% Cu sample, while the minimum wear rate (Ws = 1.06. E−4mm3/N/m) was achieved for the 4% Cu sample.

Heterogeneous carbon coated resin-based hard carbon anode material for high-performance sodium ion batteries

Resin-based hard carbons are promising anode materials for sodium ion batteries (SIBs) due to their high storage capacity and purity. However, the low initial coulombic efficiency (ICE) still hinders their practical application. Crosslinking and high-temperature pyrolysis strategies have been demonstrated to improve ICE effectively, but the complex process and high energy consumption hinder their industrialization. This paper proposes a facile synthesis of resin-based hard carbon with a soft carbon coating strategy to improve ICE. By carbonizing commercial phenolic resin at 1150℃, hard carbon with a reversible capacity of 291.6 mAh g−1 and 82.6 % ICE was obtained. After asphalt-based soft carbon coating, the optimized sample (CHC-1150) with a heterogeneous carbon coating layer of about 8.5 nm displays a high reversible capacity and ICE of 309.8 mAh g−1 and 88.2 %. Moreover, when combined with NaFe1/3Ni1/3Mn1/3O2 cathode, the assembled 18650 cylindrical-type batteries deliver a high ICE of 84.3 %, excellent low-temperature capability and cycling stability. Additionally, the disassembly results after cycling indicate that the soft carbon layer can inhibit the decomposition of electrolytes and avoid sodium plating. These encouraging results suggest that heterogeneous carbon coating should be a promising strategy to promote the electrochemical performance of resin-based hard carbon anode materials for SIBs.

Achieving a Rapid Na+ Migration and Highly Reversible Phase Transition of NASICON for Sodium-Ion Batteries with Suppressed Voltage Hysteresis and Ultralong Lifespan.

Sodium ion batteries have attracted great attention for large scale energy storage devices to replace lithium-ion batteries. As a promising polyanionic cathode material of sodium-ion batteries, Na3V2(PO4)2F3 (NVPF) belonging to NASICON exhibits large gap space and excellent structural stability, leading to a high energy density and ultralong cycle lifespan. To improve its stability and Na ion mobility, K+ cations are introduced into NVPF crystal as in situ partial substitution for Na+. The influence of K+ in situ substitution on crystal structure, electronic properties, kinetic properties, and electrochemical performance of NVPF are investigated. Through ex situ examination, it turns out that K+ occupied Na1 ion, in which the K+ does not participate in the charge-discharge process and plays a pillar role in improving the mobility of Na+. Moreover, the doping of K+ cation can reduce the bandgap energy and improve the electronic conductivity. Besides, the optimal K+ doping concentration in N0.92K0.08VPF/C is found so as to achieve rapid Na+ migration and reversible phase transition. The specific capacity of N0.92K0.08VPF/C is as high as 128.8 mAh g-1 at 0.2 C, and at 10 C its rate performance is excellent, which shows a capacity of 113.3 mAh g-1.

The effect of coprecipitation and heating temperature on structural evolution and electrochemical performance of iron-based prussian blue analogs

The effect of coprecipitation and heating temperature on structural evolution and electrochemical performance of iron-based prussian blue analogs

Rational Construction of a 3D Self-Supported Electrode Based on ZIF-67 and Amorphous NiCoP for an Enhanced Oxygen Evolution Reaction.

The development of efficient and Earth-abundant electrocatalysts for the oxygen evolution reaction (OER) is an urgent requirement in the field of electrochemical water splitting. The electrocatalytic performance of the OER can be greatly enhanced by the synergistic combination of zeolite imidazolate frameworks (ZIFs) and transition-metal phosphides, both of which individually exhibit promising capabilities in this regard. In this study, a novel amorphous NiCoP deposited on ZIF-67 sheets supported on Ni foam (labeled as NiCoP/ZIF-67/NF) as an OER electrocatalytic material was successfully synthesized using a simple, secure, and time-efficient two-step strategy. The experimental results demonstrate that NiCoP/ZIF-67/NF possesses a large active surface area with abundant active sites. Also, the synergistic effect and interaction between NiCoP and ZIF-67, as well as between Ni and Co within NiCoP, effectively enhance its electrochemical performance under alkaline conditions. Consequently, NiCoP/ZIF-67/NF exhibits outstanding catalytic activity for OER with an overpotential (η) of 175 mV at a current density of 10 mA cm-2 and a long-term stability over 40 h at 20 mA cm-2 in a 1.0 M KOH electrolyte. The corresponding analyses suggest that the real active sites responsible for the OER are identified as NiOOH and CoOOH species within the structure of NiCoP/ZIF-67/NF. Additionally, the catalytic function and stability of ZIF-67 toward the OER under alkaline conditions were also briefly discussed. This work provides a novel catalytic material for the OER along with a facile strategy to fabricate superior, efficient, and noble metal-free catalysts suitable for energy-related applications.

In-situ construction of Ni–Fe alloy nanoparticles on perovskite surface for CO2 direct electrolysis

Perovskite (ABO3) materials are commonly used as cathodes for solid oxide electrolysis cells (SOECs), but their electrochemical performance is poor due to the low CO2 adsorption and conductivity. Herein, we design an A-site deficient (La0.5Sr0.5)0.95Fe0.85Mn0.1Ni0.05O3-δ (95LSFMNi) perovskite cathode with rich oxygen vacancy and Ni–Fe alloy to enhance the CO2 adsorption. The surface precipitated Ni–Fe alloy nanoparticles introduce more oxygen vacancies into the matrix and increase the active sites for CO2 adsorption, enhancing the electrochemical reduction reaction for CO2 (CO2RR). Fe element exsolution was stimulated after the Ni reduction, and Fe content in the nanoparticles increased with the reduced time. The 95LSFMNi with in-situ dissolved Ni–Fe particles exhibits a doubled conductivity than the parent La0.5Sr0.5Fe0.9Mn0.1O3-δ (LSFM) at 800 °C and 5%H2/Ar. In addition, the electrolysis current density at 1.6 V and 800 °C reaches 1.09 A cm−2, representing a 28.2% increase compared to the LSFM. These findings demonstrate that the in-situ precipitated nano Ni–Fe particles are highly effective in enhancing the catalytic ability of CO2RR.

A facile and scalable fabrication method of scrolled graphene/boron nitride-based van der Waals superlattice heterostructure materials for highly stable supercapacitor electrode application.

Due to the increasing demand for the development of efficient renewable energy supply systems to reduce the mismatch between energy demand and utilization, supercapacitors have attracted increasing attention in the energy industry. However, the development of energy storage electrode materials to be applied at the industrial level is still challenging due to the unsatisfactory durability and scalable production issues. This study suggested a facile and scalable one-pot fabrication method of using graphene/hexagonal boron nitride (G/BN)-based one-dimensional (1D) van der Waals superlattice heterostructures (vdWSLs) as highly stable electrode materials to enhance the energy storage performance by improving the mesopore volume content, specific surface area, electrical properties, and interfacial interaction between the stacked G/BN layers. The G/BN-based vdWSLs were fabricated by a simple scrolling process through the electromagnetic interaction between the attached magnetic iron oxide nanoparticles (Fe3O4 NPs) on the surface of a G/BN vdW heterostructure (vdWH) and the applied magnetic field. The investigation results demonstrate that the changed morphology of the fabricated G/Fe/BN(NS) strongly affects the fine pore distribution, electrochemical performance, and electrical properties. Consequently, as a synergistic effect of an increased mesopore volume content, specific surface area, and C-B-N heterojunction interfacial area, the fabricated G/Fe/BN(NS) electrode showed a 100% enhancement of specific capacitance (207 F g-1 at 0.5 A g-1) and almost 7 times enhancement of electrical conductivity (800 S cm-1) with a nearly 2.3 times increase of carrier mobility (716 cm2 V-1 s-1) compared to that of the G/Fe/BN electrode. Furthermore, it exhibited outstanding long-term cycling stability with almost 119% capacitance retention even after 100 000 charge-discharge cycles. These results suggest that G/Fe/BN(NS) has tremendous potential as an electrode to fabricate high-performance supercapacitors with excellent cycling stability.

Al-Based MOF-Derived Amorphous/Crystalline Heterophase Cobalt Sulfides as High-Performance Supercapacitor Materials.

Transition metal sulfides (TMSs) are promising electrode materials due to their high theoretical specific capacitance, but sluggish charge transfer kinetics and an insufficient number of active sites hamper their applications in supercapacitors. In this work, a self-sacrificial template strategy was employed to construct Al-based MOF-derived metal sulfides with an amorphous/crystalline (a/c) heterophase, in which aluminum, nitrogen, and carbon species were evenly coordinated in the amorphous phase. The metal sulfides a/c-Co(Al)S-1 and a/c-Co(Al)S-2, originating from the CAU-1 and CoAl-MOF on NF as self-sacrificial templates, were investigated as electrode materials, respectively, in which the a/c-Co(Al)S-1 showed a more excellent electrochemical performance. Through acid etching CAU-1 using Co(NO3)2 followed by sulfuration, the a/c-Co(Al)S-1 with a unique 3D network structure was constructed, whose unique architecture expanded the interfacial contact with the electrolyte and provided vast active sites, accelerating the charge transportation and ion diffusion. Notably, the a/c-Co(Al)S-1 displayed a high specific charge of 1791.8 C g-1 at 1 A g-1, satisfactory cycle stability, and good rate capability. The corresponding assembled a/c-Co(Al)S-1//AC device delivered a high energy density of 77.1 Wh kg-1 at 800 W kg-1 and good durability (87.4% capacitance retention over 10 000 cycles).

Tailoring Alkalized and Oxidized V2CTx as Anode Materials for High-Performance Lithium Ion Batteries

V2CTx MXenes have gained considerable attention in lithium ion batteries (LIBs) owing to their special two-dimensional (2D) construction with large lithium storage capability. However, engineering high-capacity V2CTx MXenes is still a great challenge due to the limited interlayer space and poor surface terminations. In view of this, alkalized and oxidized V2CTx MXenes (OA-V2C) are envisaged. SEM characterization confirms the accordion-like layered morphology of OA-V2C. The XPS technique illustrates that undergoing alkalized and oxidized treatment, V2CTX MXene replaces -F and -OH with -O groups, which are more conducive to pseudocapacitive properties as well as Na ion diffusion, providing more active sites for ion storage in OA-V2C. Accordingly, the electrochemical performance of OA-V2C as anode materials for LIBs is evaluated in this work, showing excellent performance with high reversible capacity (601 mAh g−1 at 0.2 A g−1 over 500 cycles), competitive rate performance (222.2 mAh g−1 and 152.8 mAh g−1 at 2 A g−1 and 5 A g−1), as well as durable long-term cycling property (252 mAh g−1 at 5 A g−1 undergoing 5000 cycles). It is noted that the intercalation of Na+ ions and oxidation co-modification greatly reduces F surface termination and concurrently increases interlayer spacing in OA-V2C, significantly expediting ion/electron transportation and providing an efficient way to maximize the performance of MXenes in LIBs. This innovative refinement methodology paves the way for building high-performance V2CTx MXenes anode materials in LIBs.

Enhancing the Electrochemical Activity of 2D Materials Edges through Oriented Electric Fields.

The edges of 2D materials have emerged as promising electrochemical catalyst systems, yet their performance still lags behind that of noble metals. Here, we demonstrate the potential of oriented electric fields (OEFs) to enhance the electrochemical activity of 2D materials edges. By atomically engineering the edge of a fluorographene/graphene/MoS2 heterojunction nanoribbon, strong and localized OEFs were realized as confirmed by simulations and spatially resolved spectroscopy. The observed fringing OEF results in an enhancement of the heterogeneous charge transfer rate between the edge and the electrolyte by 2 orders of magnitude according to impedance spectroscopy. Ab initio calculations indicate a field-induced decrease in the reactant adsorption energy as the origin of this improvement. We apply the OEF-enhanced edge reactivity to hydrogen evolution reactions (HER) and observe a significantly enhanced electrochemical performance, as evidenced by a 30% decrease in Tafel slope and a 3-fold enhanced turnover frequency. Our findings demonstrate the potential of OEFs for tailoring the catalytic properties of 2D material edges toward future complex reactions.

MOF-Derived Zn/N-Doped Porous Carbon Film on a Carbon Nanotube for High-Performance Supercapacitors.

Designing high-performance binder-free electrochemical electrodes is crucially important toward supercapacitors. In this paper, a Zn/N-doped porous carbon film coating on flexible carbon nanotubes (ZIF-8@CT-800) derived from the epitaxial Zn-MOF film growth on cotton textile was successfully fabricated via a combination of the liquid-phase epitaxial (LPE) method and calcination treatments. The ZIF-8@CT-800 serves directly as a self-supported electrode for supercapacitors and exhibits a high areal capacitance of 930 mF·cm-2 at a current density of 1 mA·cm-2 and a good recyclability of 86% after 2000 cycles. The excellent supercapacitor property is ascribed to the unique structural design of ZIF-8@CT-800, which provides appropriate channels for enhanced electronic and ionic transport as well as increased surface area for accessing more electrolyte ions. This work will provide significant guidance for designing MOF-derived porous carbon to construct flexible binder-free electrode materials with high electrochemical performance.

The capacitance and shape memory effect of highly stretchable and flexible nanocomposite electrodes based on polyaniline

AbstractThe increasing demand for portable and flexible energy storage devices drives the rapid development of flexible electrodes and electrolytes. Meanwhile, the free‐standing polymer electrodes face great chance and challenge. In this work, the stretchable and flexible polyaniline/carbon nanotube/poly(vinyl alcohol) electrode (PANI/CNT/PVA‐E) was fabricated by in‐situ polymerization of aniline in CNT/PVA‐E substrate, where CNT was used to enhance the conductivity and mechanical properties of the polymer electrodes. Compared with PANI/PVA, the comprehensive performance of PANI/CNT/PVA‐E was improved. In addition, the electrochemical performance and tensile property of the electrodes depended on the CNT content. The nanocomposite electrode with 0.25% of CNT possessed optimal properties with high capacitance of 248.69 mF cm−2, and 75.29% of capacity retention over 4000 charge–discharge cycles at 1 mA cm−2. It also exhibited outstanding tensile strength of 3.88 MPa and elongation up to 462.3%. Interestingly, the electrode possessed good heat driven shape memory effect. The temporary shape could be fixed at 70°C under extra force, and the fixed shape recovered within 10 s when it was reheated to the same temperature. It is concluded that the present work may contribute to the development and fabrication of flexible energy‐storage devices, portable and highly stretchable electric devices.

Photonic Synthesis and Coating of High‐Entropy Oxide on Layered Ni‐Rich Cathode Particles

High‐entropy materials have drawn much attention as battery materials due to their distinctive properties. Lithiated high‐entropy oxide (Li0.33(MgCoNiCuZn)0.67O, LiHEO) exhibits both high lithium‐ion and electronic conductivity, making it a potential coating material for layered Ni‐rich oxide cathodes (Li1+x(Ni1−y−zCoyMnz)1−xO2, NCM or NMC) in conventional Li‐ion battery cells; however, high‐temperature synthesis limits its application. Therefore, a photonic curing strategy is used for synthesizing LiHEO and the non‐lithiated form (denoted as high‐entropy oxide [HEO]), and nanoscale coatings are successfully produced on LiNi0.85Co0.1Mn0.05O2 (NCM851005) particles. To one's knowledge, this is the first report on particle coating with high‐entropy materials using photonic curing. NCM851005 with LiHEO‐modified surface shows good cycling stability, with a capacity retention of 97% at 1 C rate after 200 cycles. The improvement in electrochemical performance is attributed to the conformal coating that prevents structural changes caused by the reaction between cathode material and liquid electrolyte. Compared to bare NCM851005, the coated material shows a significantly reduced tendency for intergranular cracking, successfully preventing electrolyte penetration and suppressing side reactions. Overall, photonic curing presents a novel cost‐ and energy‐efficient synthesis and coating procedure that paves the way for surface modification of any heat‐sensitive material for a wide range of applications.

Entropy-Assisted Anion-Reinforced Solvation Structure for Fast-Charging Sodium-Ion Full Batteries.

Anion-reinforced solvation structure favors the formation of inorganic-rich robust electrode-electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast-charging performance. Herein, a trade-off in tuning anion-reinforced solvation structure and high ionic conductivity is realized by the entropy-assisted hybrid ester-ether electrolyte. Anion-reinforced solvation sheath with more anions occupying the inner Na+ shell is constructed by introducing the weakly coordinated ether tetrahydrofuran into the commonly used ester-based electrolyte, which merits the accelerated desolvation energy and gradient inorganic-rich electrode-electrolyte interface. The improved ionic conductivity is attributed to the weakly diverse solvation structures induced by entropy effect. These enable the enhanced rate performance and cycling stability of Prussian blue||hard carbon full cells with high electrode mass loading. More importantly, the practical application of the designed electrolyte was further demonstrated by industry-level 18650 cylindrical cells.

Entropy‐Assisted Anion‐Reinforced Solvation Structure for Fast‐Charging Sodium‐Ion Full Batteries

Anion‐reinforced solvation structure favors the formation of inorganic‐rich robust electrode‐electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast‐charging performance. Herein, a trade‐off in tuning anion‐reinforced solvation structure and high ionic conductivity is realized by the entropy‐assisted hybrid ester‐ether electrolyte. Anion‐reinforced solvation sheath with more anions occupying the inner Na+ shell is constructed by introducing the weakly coordinated ether tetrahydrofuran into the commonly used ester‐based electrolyte, which merits the accelerated desolvation energy and gradient inorganic‐rich electrode‐electrolyte interface. The improved ionic conductivity is attributed to the weakly diverse solvation structures induced by entropy effect. These enable the enhanced rate performance and cycling stability of Prussian blue||hard carbon full cells with high electrode mass loading. More importantly, the practical application of the designed electrolyte was further demonstrated by industry‐level 18650 cylindrical cells.

Closed-Loop Direct Upcycling of Spent Ni-Rich Layered Cathodes into High-Voltage Cathode Materials.

Facing the resource and environmental pressures brought by the retiring wave of lithium-ion batteries (LIBs), direct recycling methods are considered to be the next generation's solution. However, the contradiction between limited battery life and the demand for rapidly iterating technology forces the direct recovery paradigm to shift toward "direct upcycling." Herein, a closed-loop direct upcycling strategy that converts waste current collector debris into dopants is proposed, and a highly inclusive eutectic molten salt system is utilized to repair structural defects in degraded polycrystalline LiNi0.83Co0.12Mn0.05O2 cathodes while achieving single-crystallization transformation and introducing Al/Cu dual-doping. Upcycled materials can effectively overcome the two key challenges at high voltages: strain accumulation and lattice oxygen evolution. It exhibits comprehensive electrochemical performance far superior to commercial materials at 4.6V, especially its fast charging capability at 15C, and an impressive 91.1% capacity retention after 200 cycles in a 1.2Ah pouch cell. Importantly, this approach demonstrates broad applicability to various spent layered cathodes, particularly showcasing its value in the recycling of mixed spent cathodes. This work effectively bridges the gap between waste management and material performance enhancement, offering a sustainable path for the recycling of spent LIBs and the production of next-generation high-voltage cathodes.