High Discharge Specific Capacity Research Articles

Rational design of low interfacial resistance between NiS2 cathode and electrolyte for high-performance Li thermal battery

As one of the main components of the cathode and electrolyte for Li thermal batteries (LTBs), conventional binders typically employ high thermal stability MgO to maintain LTBs structure stability, but MgO has the disadvantage of high resistance, which can result in a high resistance at the cathode-electrolyte interface. Thus, it is crucial to optimize the cathode-electrolyte interface for NiS2 to achieve high performance LTBs. Herein, Li7La3Zr2O12 (LLZO) with high thermal stability and excellent ionic conductivity was adopted in the cathode and electrolyte to replace the conventional binders, aiming to build a low resistance interface between the cathode and electrolyte, promoting the Li+ transport kinetics. More importantly, LLZO also plays a vital role in reducing molten salt leakage and enhancing the stability of the cathode-electrolyte interface in LTBs, which contributed to increasing the discharge capacity of the NiS2 cathode material. Consequently, LTB containing LLZO delivers a high discharge specific capacity of 635.1 mAh g−1 with a cut off voltage of 1.4 V at 100 mA cm−2 at 500 °C, retaining 72.8 % of the theoretical capacity of NiS2, which is 25.5 % higher than LTB with MgO. These findings indicate that optimizing the NiS2 electrode and LLZO electrolyte interface would be an effective way to enhance the performance of LTBs.

Copper/cobalt metal-organic framework composites for advanced anode material of lithium-ion battery

In this paper, two new types of metal-organic frameworks (MOFs) materials, namely Cu-IM and Co-MOF, have been successfully applied to the anode of lithium-ion batteries with LiPF6 (EC: DMC = 1:1, volume) electrolyte additive. Cu-IM and Co-MOF employed imidazole (IM) and 2-methylimidazole (2-MeIM) as organic ligands, respectively. The results revealed the synthesized MOFs exhibited high initial discharge specific capacities (Cu-IM: 1964.5 mAh g−1, Co-MOF: 1423.3 mAh g−1) as well as low internal resistances (Cu-IM: 146 Ω; Co-MOF: 236 Ω). To alleviate the issue of capacity decay in single MOFs, we attempted the dual-MOFs materials through the rational design of interfacial/surface properties and microstructure. Compared to Cu-IM, the prepared Cu-IM/Co-MOF composites have a higher specific surface area and pore volume. Furthermore, the charge transfer resistance of Cu-IM/Co-MOF composites (141 Ω) was lower than that of Cu-IM and Co-MOF respectively. After a heat treatment to Cu-IM/Co-MOF composites, the electrochemical performance of obtained Cu-IM/Co-MOF 250 dual-MOFs composites have been significantly improved. The Cu-IM/Co-MOF 250 dual-MOFs composites demonstrated excellent cycling stability and high discharge specific capacities at various current densities. The composites displayed stable discharge specific capacity retention of 834 mAh g−1 (50 mA g−1, 75 cycles), 710.5 mAh g−1 (200 mA g−1, 50 cycles), and 392.5 mAh g−1 (500 mA g−1, 50 cycles), highlighting their promising performance for energy storage applications. The synthesized Cu-IM/Co-MOF 250 dual-MOFs composites demonstrates exceptional cycling performance and rate capability, implying that it has the promising prospects as anode material for lithium-ion batteries.

Ultrafine Ru nanoparticles anchored on N-doped mesoporous hollow carbon spheres as a highly efficient bifunctional catalyst for Li–CO2 batteries

Rechargeable Li–CO2 battery is a facilitative and promising device for the conversion of CO2 to electrochemical energy. However, it remains a challenge to enhance the sluggish decomposition kinetics of lithium carbonate as the discharge product. Herein, the Ru nanoparticles anchored on N-doped mesoporous hollow carbon nanospheres (Ru-AHCNs) are designed as cathode to enhance the electrochemical performance of Li–CO2 battery. The Ru-AHCNs cathode displays a high discharge specific capacity of 11194.4 mA h g−1 at the current density of 100 mA g−1. In addition, the Ru-AHCNs cathode can stably run over 50 cycles and maintain a small overpotential (<1.38 V) with a limited capacity of 1000 mA h g−1 at 100 mA g−1. The excellent stability and catalytic activity of the cathode are ascribed to the following factors: (i) Uniform deposition of Ru nanoparticles in hollow carbon nanospheres can enhance the decomposition of Li2CO3 and provide considerable exposure to active sites. (ii) N-doped mesoporous hollow carbon nanospheres can provide abundant electron transport channels and promote the nucleation of discharge products. These results evidently prove the reversible formation and decomposition of the discharge products, indicating that Ru-AHCNs cathode possesses excellent bifunctional catalytic activity.

MoS2/ReS2 Hollow Heterojunction for Enhanced Aqueous Zinc-Ion Storage Performance.

The research of cathode materials for water-based zinc ion batteries (ZIBs) is very hot because the current mainstream electrode makes it difficult to meet the requirements of high specific discharge capacity and maintain a stable structure in the electrochemical process. In this work, the cathode properties are adjusted by the modification idea of morphology regulation and heterojunction construction. The simple hydrothermal method is used to prepare the hollow bimetallic heterojunction nanospheres, and their electrochemical properties as cathode materials for ZIBs are studied for the first time. Herein, the optimized cathode delivers high-rate performance and long-term cycling stability (∼98.9% Coulombic efficiency at 0.1 A g-1 after 200 cycles). The results indicate that the hollow bimetallic heterojunction nanospheres can support the material structure and provide a wide Zn2+ migration channel. The excellent performance is because hollow heterojunction bimetallic sulfides can provide abundant catalytic active sites, improve the mobility of electrons, and enhance the battery performance fundamentally. Therefore, we firmly believe that the combination of the different modification ideas can coordinate to adjust the electrode performance of ZIBs, enriching the electrode types and expanding the energy system application range.

Al-doped flower-like VO2(B) microspheres as high-performance cathode materials for lithium-ion batteries

VO2(B), as a potential cathode material for lithium-ion batteries (LIBs), is attracting extensive attention from researchers because of its great superiority in terms of theoretical specific capacity, energy density, and cost. Nevertheless, VO2(B), leads to irreversible decay of specific capacity during cycling for reasons including structural stability and inferior electrical conductivity. In this work, the electrochemical performance of VO2(B) electrode materials are further enhanced via Al ion doping. The results reveal that the prepared Al-doped 3D flower-like VO2(B) microspheres exhibit a high initial discharge specific capacity (as high as 314.8 mAh/g at 0.1 A/g current density) at an Al doping amount of n(Al3+)/n(V5+) = 6.0 %. Moreover, it displays a first discharge specific capacity of up to 229.2 mAh/g at a current density of 1 A/g with the capacity retention rate of 90.0 % after 120 cycles. As a result, Al-doped 3D flower-like VO2(B) microspheres provide enormous commercialization potential as cathode materials for LIBs.

Conjugation and Topology Engineering of 2D π-d Conjugated Metal-Organic Frameworks for Robust Potassium Organic Batteries.

The evolution of two-dimensional conjugated metal-organic frameworks (2D c-MOFs) provides a significant prospect for researching the next generation of green and advanced energy storage systems (ESSs). Especially, conjugation and topology engineering serve as an irreplaceable character in adjusting the electrochemical properties of ESSs. Herein, we proposed a novel strategy using conjugation and topology engineering to demonstrate the application of 2D c-MOFs in robust potassium-ion batteries (PIBs) for the first time. By comparing 2D c-MOFs with the rhombus/kagome structure as well as three/four-arm core, the rhombus structure (sql-Cu-TBA-MOF) cathode for PIBs can display the impressive electrochemical performance, including a high specific discharge capacity of 178.4 mAh g-1 (at 0.2 A g-1) and a well long-term cycle stability of more than 9,000 (at 10.0 A g-1). Moreover, full PIBs (FPIBs) are constructed by pairing sql-Cu-TBA-MOF cathode with dipotassium terephthalate (KTP) anode, which delivers a high reversible discharge specific capacity of 146.6 mAh g-1 (at 0.1 A g-1) and great practical application prospect. These findings provide reasonable implications for the design of 2D c-MOFs from the perspective of conjugation and topology engineering for advanced energy storage systems.

Integrating p-type phenazine into covalent triazine framework to achieve co-storage of cations and anions for quasi-solid-state dual-ion batteries

Covalent triazine frameworks (CTFs) with bipolar features have garnered significant attentions in energy storage systems. Further, the integration of p-type active sites into CTFs is highly desirable. Herein, we integrated p-type phenazine into CTFs (PZ-CTF) to generate dual active centers with ion co-storage mechanism. Interestingly, the application of PZ-CTF as the cathode material in various battery systems was demonstrated. In lithium-based dual-ion batteries (LDIBs) with liquid electrolyte, PZ-CTF can show high discharge specific capacity (190.8 mAh g−1 at 200 mA g−1) and excellent rate capability (92.8 mAh g−1 at 3000 mA g−1). In quasi-solid-state LDIBs, PZ-CTF can possess high discharge specific capacity (187.5 mAh g−1 at 200 mA g−1) and long-cycle stability (at 500 mA g−1 over 1000 cycles). In addition, in graphite-based DIBs (GDIBs), PZ-CTF also shows considerable electrochemical properties. Moreover, the continuous co-storage mechanism of PF6− and Li+ in PZ-CTF was confirmed by the theoretical calculations and spectral characterizations. This work opens a new avenue for integrating multi-polar organic electrode materials with multiple reaction mechanisms for the application of various battery systems.

An integrated electrode material based on corn straw cellulose biochar with three-dimensional network porous structure for boosting electrochemical performance of lithium batteries

In this work an integrated electrode material based on the VS4 nanoparticles grow on three-dimensional network porous biochar is put forward, forming a heterostructure that significantly boost the rate and cycle performance in lithium batteries. Biochar derives from two-steps treatment removing partial cellulose and hemicellulose, possessing three-dimensional network porous structure and naturally nitrogenous. The integrated electrode material constructs the continuous electrons transfer network, accommodates the volume expansion and traps the polar polysulfides efficiently. After 100 cycles at 1C, the integrated electrode with biochar shows the highest specific discharge capacity. Even at 2C, the three-dimensional electrode can display a high specific discharge capacity of 798.6 mAh·g−1. Thus, our study has pointed the innovations approach of constructing integrated electrode materials with porous structure biochar to enhance the electrochemical performance of lithium batteries.

Boosting sodium-ion battery performance with binary metal-doped Na3V2(PO4)2F3 cathodes

Na3V2(PO4)2F3 (NVPF), recognized for its Na superionic conductor architecture, emerges as a promising candidate among polyanion-type cathodes for sodium ion batteries (SIBs). However, its adoption in practical applications faces obstacles due to its inherently low electronic conductivity. To address this challenge, we employ a binary co-doped strategy to design Na3.3K0.2V1.5Mg0.5(PO4)2F3 cathode with nitrogen-doped carbon (NC) coating layer. This configuration enhances electronic conductivity and reduces diffusion barriers for sodium ion (Na+). The strategy of incorporating nitrogen-doped carbon coating not only facilitates the formation of a porous structure but also introduces additional defects and active sites. Such modifications accelerate the reaction kinetics and augment electrolyte interaction through an expanded specific surface area, thus streamlining the electrochemical process. Concurrently, strategic heteroatom substitution leads to a more efficient engagement of Na+ in the electrochemical activities, thereby bolstering the cathode's structural integrity. The vanadium fluorophosphate Na3.3K0.2V1.5Mg0.5(PO4)2F3@NC exhibits an electrochemical performance, including a high discharge specific capacity of 124.3 mA h g−1 at 0.1C, a long lifespan of 1000 cycles with a capacity retention of 93.1 % at 10C, and a rate property of 73.2 mA h g−1 at 20C. This research provides a method for preparing binary doped NVPF for energy storage electrochemistry.

Amorphous nanoscale antimony-vanadium oxide: A high capacity anode material for potassium ion batteries

Antimony (Sb)-based materials, as a kind of potential high capacity and low cost materials, are the focus of attention in the anode materials of potassium ion batteries. However, at present, studies on Sb-based anode materials mainly focus on Sb metal, Sb alloy and Sb chalcogenides, while reports on Sb-based oxides are relatively rare. In addition, the development of Sb-based materials is limited by their large volume variation and poor reaction kinetics for potassium storage. Herein, a novel amorphous Sb2VO5 (A-SbVO) as bimetallic antimony vanadium oxide has been synthesized by solvothermal method. The A-SbVO exhibits high K storage activity and capacity due to its nanoscale and amorphous structure. Moreover, ex-situ transmission electron microscopy and X-ray photoelectron spectroscopy revealed the evolution of the A-SbVO in the potassium storage process as follows: A-SbVO → Sb → K3Sb → Sb → Sb + Sb2VO5. After compounding with reduced graphene oxide (rGO), the as-prepared A-SbVO/rGO shows better K storage stability, with discharge specific capacities of 313.0 and 248. 8 mAh/g at 500 and 1000 mA g−1, respectively. After 300 cycles at 200 mA g−1, the A-SbVO/rGO still has a high discharge specific capacity of 382.1 mAh/g.

Intralayer ordered structure engineering for long-life Mn-based potassium-ion battery cathodes

Mn-based layered oxides have become one of the most promising cathode materials in potassium-ion batteries (PIBs) due to their high theoretical specific capacity. Nonetheless, the Jahn-Teller effect of Mn3+ leads to lattice distortion and a high K+ migration barrier, resulting in structural instability during the charge/discharge processes. To effectively overcome these problems, this work provides a method to change electronic energy levels to suppress the Jahn-Teller effect through the synergistic regulation of multiple specific element doping. The X-ray diffraction pattern of K0.4Mn0.7Ti0.1Ni0.1Cu0.1O2 shows its P3-type structure. The electrochemical test results demonstrate that K0.4Mn0.7Ti0.1Ni0.1Cu0.1O2 exhibits superior rate capacity, higher discharge specific capacity, and significant cycling stability (with a capacity retention rate of 80 % after 860 charge/discharge cycles). The in-situ X-ray diffraction pattern demonstrates the high reversibility of the electrochemical process of K+ insertion/extraction. First-principles calculations have confirmed that the electronic energy levels of K0.4Mn0.7Ti0.1Ni0.1Cu0.1O2 have better dispersion, the K+ migration channel has been effectively optimized, and the K+ migration barrier has been reduced. This study provides a significant and effective reference for the design of advanced PIBs with high performance.

Oxygen‐Poor Amorphous Heterostructure Derived from Nb2CTx Toward Superior Lithium‐Ion Storage

AbstractDue to the long‐range atomic disorder and more active sites, amorphous MXenes with better chemical reactivity and electrical conductivity, have attracted wide attention in energy storage devices. However, to reach the practical applications of MXenes, investigations into the best structure of the amorphous layer are essential. Here, the structure evolution of MXenes induced from ammonium persulfate is explored via synchrotron radiation X‐ray absorption spectroscopy. Then, a kind of oxygen‐poor amorphous heterojunction Nb2CTx MXene (a‐Nb2CTx) is designed. Benefitting from the oxygen‐poor amorphous heterojunction, the a‐Nb2CTx electrode exhibits excellent Li+ storage performance with a high discharge specific capacity of 382 mAh g−1 at 0.1 A g−1 and a long cycling stability of 300 mAh g−1 at 1.0 A g−1 after 800 cycles. Operando synchrotron X‐ray diffraction results reveal that oxygen‐poor amorphous heterojunction stabilizes Nb2CTx MXene from undergoing structural changes during cycling. This work provides new insights into the rational design of novel amorphous MXenes, which is of great significance for the development of MXenes and their applications in high‐performance energy storage systems.

Enhancing rate and stability performance of O3-type NiFeMnTi-based layered oxides via Sb/Co dual-doping

O3-type layered metal oxides have been consider as a highly suitable cathode materials for Na-ion batteries (SIBs) due to their distinct advantages of high capacity, simple synthesis and affordable price. Nonetheless, the rapid capacity attenuation and the sluggish Na+ diffusion kinetic seriously impede their practical application. Herein, a dual-doping strategy of incorporating Stibium (Sb) and cobalt (Co) elements to a quaternary oxide cathode material (Na(Ni0.3Fe0.2Mn0.5)0.9Ti0.1O2) was proposed to further ameliorate the rate capability and the cycle stability. Because of the enlarged Na and TM interlayer spacing, Sb/Co dual-doping is verified to provide a higher Na+ diffusion rate and a more stable structure. Furthermore, Co doping is found to inhibit the formation of Ni2O3 and Na0.7MnO2 impurities triggered by Sb doping. The modified Na(Ni0.3Fe0.2Mn0.5)0.8Ti0.1Sb0.05Co0.05O2 electrode represents a high discharge specific capacity of 171.6 mAh g-1 at 0.1C within the voltage range from 2.0 V to 4.3 V, and an excellent rate capability of 82.0 mAh g-1 at 5C. More significantly, it shows a splendid capacity retention of 74.69 % over 300 cycles at 1C.

An in-situ cross-linked network PMMA-based gel polymer electrolyte with excellent lithium storage performance

Gel polymer electrolytes (GPEs) effectively combine the advantages of high ionic conductivity and reduce the risk of leakage associated with liquid. In this study, a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate (PMMA) as a matrix and neopentyl glycol diacrylate (NPGDA) as cross-linking agent. The cross-linked structure of the GPE was preliminarily investigated, as well as the influence of the degree of cross-linking on its physical properties. The GPE exhibited a superior conductivity of 1.391 mS cm−1 at 25 °C. Herein, the Li|GPE|LiNi0.8Co0.1Mn0.1O2 cell has an excellent capacity retention rate of 80.7% after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g−1. The structure of the cathode material is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.

A three-dimensional co-continuous network structure polymer electrolyte with efficient ion transport channels enabling ultralong-life all solid-state lithium metal batteries

Solid polymer electrolytes (SPEs) have emerged as one of the most promising candidates for the construction of solid-state lithium batteries due to their excellent flexibility, scalability, and interface compatibility with electrodes. Herein, a novel all-solid polymer electrolyte (PPLCE) was fabricated by the copolymer network of liquid crystalline monomers and poly(ethylene glycol) dimethacrylate (PEGDMA) acts as a structural frame, combined with poly(ethylene glycol) diglycidyl ether short chain interspersed serving as mobile ion transport entities. The preparaed PPLCEs exhibit excellent mechanical property and outstanding electrochemical performances, which is attributed to their unique three-dimensional co-continuous structure, characterized by a cross-linked semi-interpenetrating network and an ionic liquid phase, resulting in a distinctive nanostructure with short-range order and long-range disorder. Remarkably, the addition of PEGDMA is proved to be critical to the comprehensive performance of the PPLCEs, which effectively modulates the microscopic morphology of polymer networks and improves the mechanical properties as well as cycling stability of the solid electrolyte. When used in a lithium-ion symmetrical battery configuration, the 6 wt%-PPLCE exhibites super stability, sustaining operation for over 2000 h at 30 °C, with minimal and consistent overpotential of 50 mV. The resulting Li|PPLCE|LFP solid-state battery demonstrates high discharge specific capacities of 160.9 and 120.1 mA h g−1 at current densities of 0.2 and 1 C, respectively. Even after more than 300 cycles at a current density of 0.2 C, it retaines an impressive 73.5% capacity. Moreover, it displayes stable cycling for over 180 cycles at a high current density of 0.5 C. The super cycle stability may promote the application for ultralong-life all solid-state lithium metal batteries.

Research on Sodium Storage Performance of Cu and Mg Doped P2 Type Layered Oxide Cathode Materials

The P2-type Ni–Mn-based oxide cathode materials have drawbacks such as the Jahn-Teller effect and crystal phase transition under high pressure. In this study, Cu and Mg modifications were introduced to inhibit the P2–O2 phase transition and increase the lattice spacing, thereby reducing the resistance of sodium ion de-embedding and intercalation to improve the overall electrochemical performance of the battery. A series of P2-type Na0.67Ni0.33−xMn0.67CuxO2 and Na0.67Ni0.33−xMn0.67MgxO2 cathode materials were synthesized through solid-state reaction. Cu substitution significantly alters the structural stability and electrochemical properties. In the voltage range from 1.5 V to 4.2 V and at 0.1 C, the initial discharge specific capacity of Na0.67Ni0.18Mn0.67Cu0.15O2 was 167 mAh·g−1, with 86 mAh·g−1 remaining after 100 cycles at 1 C. Additionally, a high discharge specific capacity of 207 mAh·g−1 was achieved with 0.075 Mg doping, suggesting that part of O2− participated in the internal electrochemical reaction. Furthermore, the rate performance of Na0.67Ni0.28Mn0.67Mg0.05O2 was found to be the best. This phenomenon was attributed to the inactive Mg2+ retaining more Na+ in the interlayer, inhibiting crystal structure transformation and Jahn-Teller distortion. The larger radius of Mg2+ increased the layer spacing, widened the Na+ de-embedding channels, and increased the diffusion coefficient.

Vertically-Aligned Card-House Structure for Composite Solid Polymer Electrolyte with Fast and Stable Ion Transport Channels.

All-solid-state lithium batteries (ASSLBs) are highly promising as next-generation energy storage devices owing to their potential for great safety and high energy density. This work demonstrates that composite solid polymer electrolyte with vertically-aligned card-house structure can simultaneously improve the high rate and long-term cycling performance of ASSLBs. The vertical alignment of laponite nanosheets creates fast and uniform Li+ ion transport channels at the nanosheets/polymer interphase, resulting in high ionic conductivity of 8.9 × 10-4 S cm-1 and Li+ transference number of 0.32 at 60°C, as well as uniformly distributed solid electrolyte interphase. Such electrolyte is characterized by high mechanical strength, low flammability, excellent structural stability and stable ion transport channels. In addition, the ASSLB cell with the electrolyte and LiFePO4 cathode delivers a high discharge specific capacity of 124.8 mAh g-1 , which accounts for 85.6% of its initial capacity after 500 cycles at 1C. The reasonable design through structural control strategy by interconnecting the vertically-aligned nanosheets open a way to fabricate high performance composite solid polymer electrolytes.

Volume contractible Antimony bromide electrode as negative electrode for long-lasting Li-ion batteries

Antimony is one of the promising anode materials for lithium-ion batteries due to its high volumetric and gravimetric capacity (theoretical specific capacity 660 mAh g-1) and stable voltage window (0.87-0.91V vs Li/Li+). However, a high-volume expansion ( ∼130%) of Sb on lithiation degrades the electrochemical performance and restricts its application. In this work, a novel strategy is explored to use antimony halide (SbBr3) instead of Sb as the starting anode material. In the first step, Li will react with SbBr3 to form LiBr and pure Sb, leading to a 78% contraction in volume, and then this pure Sb further lithiates to form Li3Sb expanding the volume (of the lithiated Sb by 130%). LiBr, which is a byproduct of the first reaction, dissolves into the solvent, leaving a porous Sb. In a nutshell, the two-step lithiation process results in a net volume-contacted porous antimony, ideal as an electrode to counter volumetric stress in subsequent charge-discharge cycles. The electrochemical performance of this electrode is much superior when compared with the pure antimony electrode, taking advantage of initial volume reduction and porous scaffold. It achieves a high specific discharge capacity of 345 mAh g-1 at a rate of 100mAg-1 even after the end of the 100th cycle and losing only 20% of its capacity. This shows that this volume contractible technique can be successfully employed for metals and metallic alloys having drastically higher Li-storing capacities than graphite.

Engineering Defect‐Rich Bimetallic Telluride with Dense Heterointerfaces for High‐Performance Lithium–Sulfur Batteries

AbstractRechargeable lithium–sulfur (Li–S) batteries have received ever‐increasing attention owing to their ultrahigh theoretical energy density, low cost, and environmental friendliness. However, their practical application is critically plagued by the sluggish reaction kinetics, shuttling of soluble polysulfide intermediates, and uncontrollable growth of Li dendrites. Herein, a bimetallic telluride electrocatalyst with dense heterointerfaces and rich defects embedded in hollow carbon polyhedron bunches (N⊂CoTe1‐x/ZnTe1‐y@NC, abbreviated as NCZTC) is rationally designed to simultaneously address the S cathode and Li anode problems. Both experimental and computational results substitute the integration of dense heterointerfaces and rich defects can synergistically modulate the electronic structure, enhance the electrical conductivity, promote the Li+ transportation, strengthen the polysulfides adsorption and improve the catalytic activity, thereby significantly accelerating the redox conversion kinetics and prevent the dendrite growth. Consequently, Li–S batteries with NCZTC‐modified separators demonstrate excellent electrochemical performance including high specific discharge capacity, remarkable rate capability, good long‐term cycling stability, and competitive areal capacity even at high sulfur loading and lean electrolyte conditions. This study not only provides valuable guidance for designing efficient sulfur electrocatalysts with transition metal tellurides but also emphasizes the importance of heterostructure design and defect engineering for high‐performance Li–S batteries.

Scalable direct recycling of spent LiNi1/3Co1/3Mn1/3O2 via in-situ elements replenishment and structural restoration

The proliferation of vehicles and portable devices has led to a significant increase in the number of spent lithium-ion batteries (LIBs). Recycling these spent LIBs is crucial to prevent negative environmental impacts and resource wastage. However, traditional pyrometallurgical and hydrometallurgical methods suffer from inherent drawbacks as being time-consuming, energy-intensive and causing secondary pollution. Herein, an innovative approach is proposed to direct regenerate degraded LiNi1/3Co1/3Mn1/3O2 (NCM111) in-situ by combining hydrothermal treatment with solid-state sintering. Structural and morphology characterizations reveal that the amorphous layer near the surface of degraded NCM111 (D-NCM111) are dissolved after the hydrothermal treatment, restoring the original layered structure due to the relithiation reaction, whereas the target stoichiometric ratios of transition metal elements are achieved through the solid-state sintering process. The regenerated NCM111 (R-NCM111) exhibits a high discharge specific capacity of 152.3 mAh/g at 0.1 C and a capacity retention of 96.1% at 1 C after 300 cycles. The recycling method presented in this work is not only facile but also scalable, potentially opening a new pathway to address the environmental challenges posed by massive spent LIBs.