Lithium Storage Research Articles

Tuning Work Function of Fe2N@C Nanosheets by Co Doping for Enhanced Lithium Storage.

Transition metal nitrides (TMNs) with high theoretical capacity and excellent electrical conductivity have great potential as anode materials for lithium-ion batteries (LIBs), but suffer from poor rate performance due to the slow kinetics. Herein, taking the Fe2N for instance, Co doping is utilized to enhance the work function of Fe2N, which accelerates the charge transfer and strengthens the adsorption of Li+ ions. The Fe2N nanoparticles with various Co dopants are anchoring on the surface of honeycomb porous carbon foam (named Cox-Fe2N@C). Co-doping can enlarge the work function of pristine Fe2N and thereby optimize the charging/discharging kinetics. The work function can be increased from 5.23eV (pristine Fe2N) to 5.67eV for Co0.3-Fe2N@C and 5.56eV for Co0.1-Fe2N@C. As expected, the Co0.1-Fe2N@C electrode exhibits the highest specific capacity (673mA h g-1 at 100mA g-1) and remarkable rate capability (375mA h g-1 at 5000mA g-1), outperforming most reported TMNs electrodes. Therefore, this work provides a promising strategy to design and regulate anode materials for high-performance and even commercially available LIBs.

Identification of carbon-wrapped Bi5Nb3O15 as a viable intercalation/alloying high-performance lithium storage material

Identification of carbon-wrapped Bi5Nb3O15 as a viable intercalation/alloying high-performance lithium storage material

Enhancing the Lithium Storage Performance of Phosphorus–Carbon Composites by Reinforcing P–C Bonding with High-Strength Metal Nanoparticles

Enhancing the Lithium Storage Performance of Phosphorus–Carbon Composites by Reinforcing P–C Bonding with High-Strength Metal Nanoparticles

Anthracite-Derived Porous Carbon@MoS2 Heterostructure for Elevated Lithium Storage Regulated by the Middle TiO2 Layer.

The rational design of MoS2/carbon composites have been widely used to improve the lithium storage capability. However, their deep applications remain a big challenge due to the slow electrochemical reaction kinetics of MoS2 and weak bonding between MoS2 and carbon substrates. In this work, anthracite-derived porous carbon (APC) is sequential coated by TiO2 nanoparticles and MoS2 nanosheets via a chemical activation and two-step hydrothermal method, forming the unique APC@TiO2@MoS2 ternary composite. The dynamic analysis, in-situ electrochemical impedance spectroscopy as well as theoretical calculation together demonstrate that this innovative design effectively improves the ion/electron transport behavior and alleviates the large volume expansion during cycles. Furthermore, the introduction of middle TiO2 layer in the composite significantly strengthens the mechanical stability of the entire electrode. As expected, the as-prepared APC@TiO2@MoS2 anode displays a high lithium storage capacity with a reversible capacity of 655.8 mAh g-1 after 150 cycles at 200 mA g-1, and robust cycle stability. Impressively, even at a high current density of 2 A g-1, the electrode maintains a superior reversible capacity of 597.7 mAh g-1 after 1100 cycles. This design highlights a feasibility for the development of low-cost anthracite-derived porous carbon-based electrodes.

Multi-Scale Risk-Informed Comprehensive Assessment Methodology for Lithium-Ion Battery Energy Storage System

Lithium-ion batteries (LIB) are prone to thermal runaway, which can potentially result in serious incidents. These challenges are more prominent in large-scale lithium-ion battery energy storage system (Li-BESS) infrastructures. The conventional risk assessment method has a limited perspective, resulting in inadequately comprehensive evaluation outcomes, which impedes the provision of dependable technical support for the scientific appraisal of intricate large-scale Li-BESS systems. This study presents a novel Li-BESS-oriented multi-scale risk-informed comprehensive assessment framework, realizing the seamless transmission of assessment information across various scales. The findings from a previous smaller-scale analysis serve as inputs for a larger scale. The evaluation process of this method is more scientifically rigorous and yields more comprehensive results compared to assessment technologies just relying on a single perspective. By utilizing the proposed comprehensive assessment methodology, this study utilized the emergency power supply of nuclear power plants (NPPs) as an application scenario, demonstrating the complete implementation process of the framework and conducting a comprehensive assessment of Li-BESS feasibility as an emergency power source for NPPs. Our findings propose a novel paradigm for the comprehensive assessment of Li-BESS, which is expected to serve as a scientific foundation for decision-making and technical guidance in practical applications.

Structurally-constrained wrinkled NiO nanomembranes for high-performance lithium and sodium storage

In light of its exceptional capacity and safety features, nickel oxide (NiO) has emerged as a highly promising electrode material for advanced lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), which operate through conversion mechanisms, meeting the growing demand for high-efficiency rechargeable batteries. To address the capacity degradation challenges associated with NiO anodes, we present an innovative approach involving the fabrication of wrinkled NiO nanomembranes through magnetron sputtering deposition followed by thermal treatment. This distinctive three-dimensional, ultra-thin architecture integrates nanostructural and microstructural features that effectively reduce ionic diffusion distances and mitigate dimensional fluctuations during cycling, thereby markedly enhancing the electrochemical performance and reliability. Specifically, for lithium storage, these wrinkled NiO nanomembranes achieve an impressive reversible specific capacity of 773 mA h g−1 at 100 mA g−1, with excellent rate capability of 468 mA h g−1 at 5000 mA g−1 and long-term cycling performance, maintaining 523 mA h g−1 at 500 mA g−1 even after 1000 cycles. Likewise, for sodium storage, they exhibit a substantial reversible capacity of 288 mA h g−1 at 50 mA g−1 and retain 202 mA h g−1 at 200 mA g−1 after 100 cycles. These findings underscore the promising application of wrinkled NiO nanomembranes as robust anodic materials for high-performance LIBs and SIBs.

Nano Silicon Integrated Hard Carbon from Conjugated Microporous Polymer for High‐Efficient Lithium Storage

AbstractIt is a significant issue to develop silicon/carbon composite anode with high‐capacity and long cycling stability for lithium‐ion batteries. However, the huge volume expansion of silicon during lithiation leads to severe pulverization of silicon, resulting in serious capacity fading over cycles. Herein, nano silicon integrated hard carbon (20Si@HC, 20 wt% nano silicon) is prepared by pyrolyzing nano silicon in‐situ coated a conjugated microporous polymer (CMP). CMP‐derived hard carbon coating features developed porous structure, which not only deliver a high lithium storage capacity, but also provide enough space for the volume expansion of nano silicon. When evaluated as an anode for lithium‐ion batteries, the 20Si@HC delivers an impressive 1037 mAh g−1 at 0.1 A g−1 and a capacity retention ratio of 72.07% for 100 cycles at 0.6 A g−1, providing some reference for designing high‐capacity silicon/carbon composites.

Investigation and Optimization of Electrochemical Lithium Storage in Natural Stibnite

Investigation and Optimization of Electrochemical Lithium Storage in Natural Stibnite

Fully sp2 Carbon-Conjugated Covalent Organic Frameworks with Multiple Active Sites for Advanced Lithium-Ion Battery Cathodes.

Covalent organic frameworks (COFs) hold great promise for rechargeable batteries. However, the synthesis of COFs with abundant active sites, excellent stability, and increased conductivity remains a challenge. Here, chemically stable fully sp2 carbon-conjugated COFs (sp2c-COFs) with multiple active sites are designed by the polymerization of benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-tricarbaldehyde) (BTT) and s-indacene-1,3,5,7(2H,6H)-tetrone (ICTO) (denoted as BTT-ICTO). The morphology and structure of the COF are precisely regulated from "butterfly-shaped" to "cable-like" through an in situ controllable growth strategy, significantly promoting the exposure and utilization of active sites. When the unique "cable-like" BTT-ICTO@CNT is employed as lithium-ion batteries (LIBs) cathode, it exhibits exceptional capacity (396 mAh g-1 at 0.1 A g-1 with 97.9 % active sites utilization rate), superb rate capacity (227 mAh g-1 at 5.0 A g-1), and excellent cycling performance (184 mAh g-1 over 8000 cycles at 2.0 A g-1 with 0.00365 % decay rate per cycle). The lithium storage mechanism of BTT-ICTO is exhaustively revealed by in situ Fourier transform infrared, in situ Raman, and density functional theory calculations. This work provides in-depth insights into fully sp2c-COFs with multiple active sites for high-performance LIBs.

Fully sp2 Carbon‐Conjugated Covalent Organic Frameworks with Multiple Active Sites for Advanced Lithium‐Ion Battery Cathodes

AbstractCovalent organic frameworks (COFs) hold great promise for rechargeable batteries. However, the synthesis of COFs with abundant active sites, excellent stability, and increased conductivity remains a challenge. Here, chemically stable fully sp2 carbon‐conjugated COFs (sp2c‐COFs) with multiple active sites are designed by the polymerization of benzo[1,2‐b:3,4‐b′:5,6‐b′′]trithiophene‐2,5,8‐tricarbaldehyde) (BTT) and s‐indacene‐1,3,5,7(2H,6H)‐tetrone (ICTO) (denoted as BTT‐ICTO). The morphology and structure of the COF are precisely regulated from “butterfly‐shaped” to “cable‐like” through an in situ controllable growth strategy, significantly promoting the exposure and utilization of active sites. When the unique “cable‐like” BTT‐ICTO@CNT is employed as lithium‐ion batteries (LIBs) cathode, it exhibits exceptional capacity (396 mAh g−1 at 0.1 A g−1 with 97.9 % active sites utilization rate), superb rate capacity (227 mAh g−1 at 5.0 A g−1), and excellent cycling performance (184 mAh g−1 over 8000 cycles at 2.0 A g−1 with 0.00365 % decay rate per cycle). The lithium storage mechanism of BTT‐ICTO is exhaustively revealed by in situ Fourier transform infrared, in situ Raman, and density functional theory calculations. This work provides in‐depth insights into fully sp2c‐COFs with multiple active sites for high‐performance LIBs.

Effect of ambient pressure on the fire characteristics of lithium-ion battery energy storage container

As lithium-ion battery energy storage gains popularity and application at high altitudes, the evolution of fire risk in storage containers remains uncertain. In this study, numerical simulation is employed to investigate the fire characteristics of lithium-ion battery storage container under varying ambient pressures. The findings reveal that the peak heat release rate of fires at normal pressure is significantly higher than at lower pressure. Specifically, the heat release rate at 100 kPa is 9215 kW, exceeding the value at 40 kPa by 42%, which is only 3900 kW. This peak heat release rate also demonstrates a power function relationship with ambient pressure. In addition, fires tend to last longer in lower pressure, where high-temperature areas expand and spread rates increase. Moreover, higher pressures produce elevated peak concentrations of CO and CO2, while smoke spreads faster in lower pressure, despite lower peak smoke concentrations. The study findings can serve as a foundation for assessing the fire hazards and designing fire protection measures for lithium-ion battery storage containers exposed to varying ambient pressures.

Direct regeneration of LiFePO4 cathode by inherent impurities in spent lithium-ion batteries

The direct regeneration method, recognized for its cost-effectiveness, has garnered considerable attentions in the field of battery recycling. In this study, a novel direct regeneration strategy is proposed to repair spent LiFePO4 (S-LFP) cathodes without the need for impurity removal. Instead, the residual conductive carbon and polyvinylidene fluoride (PVDF) in S-LFP are employed as inherent reductive agents. Systematic characterization and analysis reveal that the failure of S-LFP primarily originates from a substantial loss of Li+ and the conversion of LiFePO4 to FePO4. Meanwhile, it is demonstrated that both residual conductive carbon and PVDF play positive roles in promoting the regeneration of S-LFP through distinct mechanisms. As a result, the regenerated LFP exhibits significant recovery in crystal structure and chemical composition as compared to S-LFP, which leads to notably improved lithium storage performance. Furthermore, to further enhance the lithium storage property, a specific amount of glucose (10 %) is introduced during the regeneration of S-LFP, yielding a regenerated product that performs comparably to commercial LFP. Clearly, our approach, in contrast to traditional regeneration methods, maximizes the utilization of residual impurities within S-LFP, resulting in effective regeneration of S-LFP, thereby proving both informative and cost-effective.

Quantitative pre-intercalation of alkali metal ions enables precisely modulating Li+ storage of MXenes

Ion intercalation is crucial for improving energy storage performance, but controlling the content of intercalated ions is challenging for two-dimensional (2D) electrode materials although it enables clarifying individual intercalation behaviors and thereof pinpointing the intercalation mechanism. Herein, the equal‐content alkali metal ions were successfully manipulated to intercalate into Mo2CTx MXene electrodes via an electrochemistry‐driven approach via the anti‐battery principle. Based on a variety of alkali metal ions pre‐intercalation into the Mo2CTx MXene (M+‐Mo2CTx) electrodes, the lithium storage performance was largely improved. Li+‐Mo2CTx electrode exhibits an outstanding capacity of 395.49 mAh g−1 at 200 mA g−1 after 100 cycles due to the enhanced redox activity induced by high-valence Mo and low -F interlayer exposed surface. Besides, the K+‐Mo2CTx electrode delivers excellent rate performance due to faster ion transfer kinetics originating from the pillaring effect of pre-intercalated K+ ions. In a broader sense, our study opens up a new route to accurately improve the electrochemical performance via precisely tuning the content of ions intercalated into 2D intercalation‐type materials.

Polyacrylonitrile and aluminum metal dual functionalization interconnected network for superior lithium storage in silicon anode

Currently, silicon-based anode is one of the most promising anode materials that can be applied in next-generation lithium-ion batteries. However, the high activity of the electrode–electrolyte interface and low electronic conductivity of Si anode during the cycling process greatly limits its large-scale application. Aluminum (Al) is the metallic current collector known to promote electronic conductivity and lithium-ion transfer at low cost. However, to our knowledge, scalable interface engineering incorporating Al with carbonized polymer has not been reported. Herein, a polyacrylonitrile (PAN) and aluminum metal dual functionalization interconnected network is achieved via a simple sol-gel method followed by high-temperature calcination to obtain a stable solid electrolyte interphase (SEI) while allowing fast Li+ transmission. The calculated diffusion energy barrier for lithium ions in Al is 0.2198 eV, significantly lower than that in Cu and Fe. Benefiting from the enhanced interfacial protection and kinetics of Si with polyacrylonitrile/Al, the prepared Si@Al@CPAN anode exhibits high lithium storage capacity (2034.90 mAh/g after 150 cycles at 0.84 A/g). At the same time, the prepared Si@Al@CPAN anode outperforms the pure Si anode in rate performance at 12.6 A/g (1116.75 mAh/g vs. 2.84 mAh/g). The present work delivers new design ideas for high-performance Si anode with a multi-functionalization interface.

Vertically Aligned MoS2 Nanosheets with Increased Interlayer Spacing on Hollow Polypyrrole Nanotubes for Enhanced Lithium and Sodium Storage Performance

Vertically Aligned MoS₂ Nanosheets with Increased Interlayer Spacing on Hollow Polypyrrole Nanotubes for Enhanced Lithium and Sodium Storage Performance

Element Screening Engineering for High-Entropy Alloy Anodes: Achieving Fast and Robust Li-Storage With Optimal Working Potential.

While the high-entropy strategy is highly effective in enhancing the performance of materials across various fields, an optimal methodology for selecting component elements for performance optimization is still lacking. Here the findings on uncovering the element selection rules for rational design of high-entropy alloy anodes with exceptional lithium storage performance are reported. It is investigated high-entropy element screening rules by modifying stable diamond-structured Ge with P to induce a tetrahedrally coordinated sphalerite structure for enhanced metallic conductivity, further stabilized by incorporating Zn and other elements. Moreover, both theoretical and experimental results confirm that Li-storage performance improves with increasing atomic number: BZnGeP3 < AlZnGeP3 < GaZnGeP3 < InZnGeP3. InZnGeP3-based electrodes demonstrate the highest Li-ion affinity, fastest electronic and Li-ion transport, largest Li-storage capacity and reversibility, and best mechanical integrity. Further element screening based on the above criteria leads to high entropy alloy anodes with metallic conductivity like GaCuSnInZnGeP6, GaCu(or Sn)InZnGeP5, CuSnInZnGeP5, InZnGePSeS(or Te), InZnGeP2S(or Se) which show superior Li-storage performances. The excellent phase stability is attributed to their high configurational entropy. This study offers profound insights into element screening for high-entropy alloy-based anodes in Li-ion batteries, providing guidance and reference for the element combination and screening of other high-entropy functional materials.

Recent Advances in Cost‐Effective ZnO‐Based Electrode Material for Lithium‐Ion Batteries

AbstractFuel cell and lithium ion battery (LIB) technologies are increasingly recognized as cutting‐edge power sources that are gradually displacing various versions of older systems. High‐performance electrode materials must be developed for enhanced next‐generation LIBs. Because of their low cost, high theoretical specific capacity, and environmental friendliness, nanoparticles based on zinc oxide (ZnO) have been regarded as promising alternatives. However, significant problems including intrinsic poor conductivity and significant volume expansion have made ZnO‐based nanomaterials for less viable. In this review we discussed about the mechanism of lithium ion battery and how strategies to overcome intrinsic poor conductivity and significant volume expansion of ZnO‐based nanomaterials. Followed by the best methods for improving the lithium ion storage capacity of ZnO‐based materials as cathode and anode separately reviewed. And summarized the challenges and potential lines of inquiry for Zn‐based nanomaterials in the future.

Dramatic Enhancement Enabled by Introducing TiN into Bread-like Porous Si-Carbon Anodes for High-Performance and Safe Lithium Storage.

Doping modifications and surface coatings are effective methods to slow volume dilatation and boost the conductivity in silicon (Si) anodes for lithium-ion batteries (LIBs). Herein, using low-cost ferrosilicon from industrial production as the energy storage material, a bread-like nitrogen-doped carbon shell-coated porous Si embedded with the titanium nitride (TiN) nanoparticle composite (PSi/TiN@NC) was synthesized by simple ball milling, etching, and self-assembly growth processes. Remarkably, the porous Si structure formed by etching the FeSi2 phase in ferrosilicon alloys can provide buffer space for significant volume expansion during lithiation. Highly conductive and stable TiN particles can act as stress absorption sites for Si and improve the electronic conductivity of the material. Furthermore, the nitrogen-doped porous carbon shell further helps to sustain the structural stability of the electrode material and boost the migration rate of Li-ions. Benefiting from its unique synergistic effect of components, the PSi/TiN@NC anode exhibits a reversible discharge capacity up to 1324.2 mAh g-1 with a capacity retention rate of 91.5% after 100 cycles at 0.5 A g-1 (vs fourth discharge). Simultaneously, the electrode also delivers good rate performance and a stable discharge capacity of 923.6 mAh g-1 over 300 cycles. This research can offer a potential economic strategy for the development of high-performance and inexpensive Si-based anodes for LIBs.

Coordinate regulation of amorphous carbon microspheres and crystal structure of iron oxalate for high rate lithium storage ability

Iron oxalate is one of the highly potential anode materials for lithium-ion batteries, but its widespread application is limited by slow electron transfer rate and sluggish electrochemical reactions. Herein, iron oxalate/amorphous carbon microspheres (FeC2O4/PCC) composite with uniformly mixed crystalline phase for more stable active sites and three-dimensional conductive network, was synthesized via the in-situ self-polymerization, carbonization of β-cyclodextrin and recrystallization technique under solvothermal condition. The self-aggregation progress and kinetics of recrystallization accelerate the crystalline phase transformation of iron oxalate and the morphology reconstruction of micron-grade polygonal prism particles. Based on the fast electron migration facilitated by three-dimensional conductive network of PCC and exceptionally stable structure and Li+ diffusion channels endowed by strengthening effect of recrystallization, FeC2O4/PCC-15 % exhibits long cycling life and outstanding ability for high-rate lithium storage: the specific capacities of 1231.50 and 1128.75 mAh g−1 after 500 cycles at current densities of 3 and 5 A g−1, with capacity retention rates of 90.79 % and 81.08 %, respectively. Furthermore, according to electrochemical capacity contribution analysis, PCC also can remarkably enhance the reversible lithium storage ability of interfacial capacitive effects and conversion reaction even under high current density. This work provides a new modification pathway for the application of transition metal oxalate systems in fast charging field.

Two-dimensional vanadium carbide (V2C) MXene derived heterostructures for high-performance lithium storage

Li3VO4 is notable for its high theoretical capacity and favorable lithium-ion insertion potential, making it a promising candidate for lithium storage applications. However, its practical use is limited by low electronic conductivity, which results in reduced electrochemical performance and significant resistance polarization during lithium storage. Herein, we developed a Li3VO4/V2CTx heterostructure using a MXene-derived approach, where Li3VO4 is anchored onto a conductive V2CTx MXene substrate. Theoretical calculations suggest that the heterostructure exhibits enhanced lithium adsorption capabilities compared to V2CTx, indicating improved interactions with lithium ions. The synthesized Li3VO4/V2CTx heterostructure demonstrates excellent rate performance and cycling stability. Additionally, a lithium-ion capacitor utilizing this heterostructure as the anode and activated carbon as the cathode achieves impressive power density and energy density. This study underscores the potential of this heterostructure as a high-performance anode material and offers valuable insights for the design of other advanced electrode materials.