High-rate Cycling Research Articles

Electrolyte Design via Cation-Anion Association Regulation for High-Rate and Dendrite-Free Zinc Metal Batteries at Low Temperature.

Low-temperature zinc metal batteries (ZMBs) are highly challenged by Zn dendrite growth, especially at high current density. Here, starting from the intermolecular insights, we report a cation-anion association modulation strategy by matching different dielectric constant solvents and unveil the relationship between cation-anion association strength and Zn plating/stripping performance at low temperatures. The combination of comprehensive characterizations and theoretical calculations indicates that moderate ion association electrolytes with high ionic conductivity (12.09 mS cm-1 at -40 °C) and a stable anion-derived solid electrolyte interphase (SEI) jointly account for highly reversible and dendrite-free Zn plating/stripping behavior, resulting in high-rate and ultrastable cycle performance at low temperature. As a result, at -40 °C, Zn//Zn cells can stably cycle over 400 h at 5 mA cm-2 and 10 mAh cm-2 and Zn//Cu cells exhibit an exceptional average Coulombic efficiency (CE) of 99.91% for 1800 cycles at 1 mA cm-2 and 1 mAh cm-2. Benefiting from enhanced low-temperature Zn plating/stripping performance, Zn//PANI full cells stably operate for 12,000 cycles at 0.5A g-1 and 35,000 cycles at 5 A g-1. Impressively, at -60 °C, Zn//Cu cells still display a high average CE of 99.68% for 2000 cycles. This work underscores the crucial effect of cation-anion association regulation for high-rate and dendrite-free Zn metal anodes, deepening the understanding of intermolecular interaction insights for low-temperature electrolyte design.

Quantifying Lithium-Ion Battery Rate Capacity, Electrode Structuring, and Transport Phenomena Using E-I Measurements

The specific energy of lithium-ion batteries (LIBs) can be enhanced through various approaches, one of which is increasing the proportion of active materials by thickening the electrodes. However, this typically leads to the battery having lower performance at a high cycling rate, a phenomenon commonly known as rate capacity retention. One solution to this is perforating the electrode, by creating channels or corrugations in the active electrode material, either as holes or as channels. This is known to reduce the rate capacity retention effect, but in order to engineer this better, a simplified transport process analysis needs to be established. In this paper, we propose a classic electrochemical analysis based on voltage–charge cycling measurements in order to obtain a classical mass transport coefficient, hm, that is further used as a main indicator for electrode design quality assessment. We also demonstrate theoretically and experimentally how the mass transfer coefficient, hm, can be determined and how it changes as the electrode layer thickness increases, with and without electrode corrugations.

Selection of high rate capability and cycling stability MnO anode material for lithium-ion capacitors: Effect of the carbon source

The N-doped carbon modified MnO composites were successfully prepared using K2MnO4 as the manganese source, CH4N2O as the nitrogen source, and glucose, sucrose, or reduced graphene oxide as the carbon sources. Among them, the composite (MPN) prepared using glucose as the carbon source exhibited excellent electrochemical performance, attributed to its relatively small particle size (6.4 nm), high specific surface area of 199.4 m2·g−1, and a high ID/IG ratio of 0.86. The MnO in MPN contained a significant amount of Mn3+, ∼16.8 %, which is ascribed to the incomplete reduction of high valence Mn during the process of synthesis. With the formation of Mn3+, a large number of cationic vacancies were generated, which increased the diffusion coefficient of Li+ from 2.12 × 10−14 cm2 s −1 to 5.94 × 10−13 cm2 s−1. The carbon layer with appropriate thickness, doped N and mesoporous structure suitable for electrolyte transport provide a fast ion/electron transport channels for MnO, and ensure a stable interface structure in the electrochemical reactions. Consequently, the MPN anode material exhibited remarkable high current discharge capacity (769.5 mAh·g−1 at a high current density of 2 A·g−1) and excellent cycling performance (882.2 mAh·g−1 after 200 cycles at 1 A·g−1), indicating its exceptional rate performance and cycle stability. Furthermore, the lithium ion capacitor constructed with MPN as anode and activated carbon as cathode demonstrated a high specific energy of 190 Wh·kg−1, a high specific power of 205.3 W·kg−1, and an impressive cycling lifespan of up to 3000 cycles without obvious degradation.

Tuning Crystalline Preferred Orientation of SnSe2 Anode by Co-doping to Enhance Pseudocapacitive Behaviors for High-Performance Sodium Storage.

SnSe2 has attracted great attention due to its unique 2D-layered structure, which makes it capable of sodium ion storage and higher theoretical capacities compared to traditional anode materials like hard carbon for sodium ion batteries (SIBs). However, SnSe2-based materials will cause structural damage due to volume expansion during ion storage, leading to poor cycle stability and rate capacity. In this work, Co-doped SnSe2 (Co-SnSe2) with preferred crystal orientation was fabricated by a one-step solvothermal method. It has been found that after doping Co, the lower (001) crystal plane located at 14.4° replaced the higher (101) plane at 30.7° as the dominant crystal plane in Co-SnSe2, which significantly promoted ion diffusion and enhanced the pseudocapacitance behavior. Therefore, this Co-SnSe2 anode achieves a high capacity of 504 mAh g-1 at 1 A g-1, and a high-rate cycle stability, delivering a reversible capacity of 302 mAh g-1 at 5 A g-1 after 1800 cycles with a retained capacity rate of 94%. Moreover, the Na3V2(PO4)3||Co-SnSe2 full cell exhibits a stable cycle performance of over 300 cycles at 1 A g-1, demonstrating great promise for practical applications. This work provides an effective reference for the exploration of high-performance sodium storage anode materials.

Quantitative pre-lithiation modulation of aluminum foil anode kinetics enables high rate and stable cycling of high-loading all-solid-state batteries

Aluminum (Al) foil holds great promise as a pure alloy anode for all-solid-state batteries (ASSBs) due to its suitable potential, high theoretical capacity, and excellent electronic conductivity. However, it remains challenging to achieve high reversibility and stability of the Al foil anode for ASSBs. Herein, we investigate the morphological and lithium (Li) kinetics evolutions of the Al foil anode paired with sulfide solid-state electrolyte (SSE). We identify that the significant reversible capacity loss stems from diminished Li kinetics at low Li contents (LixAl, 0 < x < 0.5), where the accumulation of pores and pure delithiated Al phase obstructs Li diffusion, increasing interfacial resistance and overpotential. Conversely, the Al foil anode with high Li contents (LixAl, 0.5 < x < 1) demonstrates reversible structures and rapid Li kinetics. Through precise pre-lithiation control, ASSBs with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes exhibit outstanding rate capabilities and cycling stability, achieving over 4,000 cycles with 82.1 % capacity retention at 5C and demonstrating long-term cycling over 1,000 cycles with nearly 100 % capacity retention at ultra-high loadings. This work offers a viable strategy for advancing practical-level ASSBs with enhanced performance and longevity, contributing valuable insights to future battery technology.

Hollow carbon nanofibers with self-induced internal electric field for high-performance full-carbon sodium ion capacitors

Self-induced internal electric field (SIEF) is crucial to achieve high capacity, high rate and long cycle life of carbon anodes in Na+ storage, but it is also a huge challenge currently. Herein, a template-assisted electrospinning process and subsequent low-temperature pyrolysis method is employed to synthesize S, N co-doped hollow carbon nanofibers (SNHCF) with rich micropores and chemisorption sites. The rich micropores and interconnected macroporous in SNHCF provide large internal availability that effectively exposing the active sites, inhibiting the volume expansion and shortening the Na+ diffusion distance. Besides, S, N co-doping in the carbon skeleton can act as an electron acceptor and electron donor respectively to form a SIEF to boost adsorption of Na+. Theoretical calculation and ex-situ characterizations confirmed that S, N co-doping can regulate the electronic configuration and reduce the diffusion barrier of Na+. As a result, SNHCF anode has ultra-high specific capacity (588.2mAh g−1 at 0.05 A/g) and impressive rate performance (264.3mAh g−1 at 20 A/g). The full-carbon sodium ion capacitors assembled with SNHCF anode and activated carbon cathode exhibits high energy density (119 Wh kg−1) and ultra-long cycle stability (80.06 % capacity retention after 12,000 cycles).

Building Li–S batteries with enhanced temperature adaptability via a redox-active COF-based barrier-trapping electrocatalyst

Covalent organic frameworks (COFs) are promising materials for mitigating polysulfide shuttling in lithium-sulfur (Li–S) batteries, but enhancing their ability to convert polysulfides across a wide temperature range remains a challenge. Herein, we introduce a redox-active COF (RaCOF) that functions as both a physical barrier and a kinetic enhancer to improve the temperature adaptability of Li–S batteries. The RaCOF constructed from redox-active anthraquinone units accelerates polysulfide conversion kinetics through reversible C=O/C-OLi transformations within a voltage range of 1.7 to 2.8 V (vs. Li+/Li), optimizing sulfur redox reactions in ether-based electrolytes. Unlike conventional COFs, RaCOF provides bidentate trapping of polysulfides, increasing binding energy and facilitating more effective polysulfide management. In-situ XRD and ToF-SIMS analyses confirm that RaCOF enhances polysulfide adsorption and promotes the transformation of lithium sulfide (Li2S), leading to better sulfur cathode reutilization. Consequently, RaCOF-modified Li–S batteries demonstrate low self-discharge (4.0% decay over a 7-day rest), excellent wide-temperature performance (stable from −10 to +60 °C), and high-rate cycling stability (94% capacity retention over 500 cycles at 5.0 C). This work offers valuable insights for designing COF structures aimed at achieving temperature-adaptive performance in rechargeable batteries.

Fast, variable stiffness-induced braided coiled artificial muscles

Biomimetic actuation technologies with high muscle strokes, cycle rates, and work capacities are necessary for robotic systems. We present a muscle type that operates based on changes in muscle stiffness caused by volume expansion. This muscle is created by coiling a mechanically strong braid, in which an elastomer hollow tube is adhesively attached inside. We show that the muscle reversibly contracts by 47.3% when driven by an oscillating input air pressure of 120 kilopascals at 10 Hz. It generates a maximum power density of 3.0 W/g and demonstrates a mechanical contractile efficiency of 74%. The muscle's low-pressure operation allowed for portable, thermal pneumatical actuation. Moreover, the muscle demonstrated bipolar actuation, wherein internal pressure leads to muscle length expansion if the initial muscle length is compressed and contraction if the muscle is not compressed. Modeling indicates that muscle expansion significantly alters its stiffness, which causes muscle actuation. We demonstrate the utility of BCMs for fast running and climbing robots.

Enhanced Cycling Performance of Spinel LiNi0.5Mn1.5O4 Cathodes through Mg-Mn Hetero-Valent Doping via Microwave Sol-Gel Method.

As a high energy density cathode material, further development of high working voltage spinel LiNi0.5Mn1.5O4 has hindered by its rapid capacity degradation. To address this, a hetero-valent substitution of magnesium for manganese was used to synthesize spinel LiNi0.5MgxMn1.5-xO4 (x = 0, 0.03, 0.05) via a microwave sol-gel method. XRD and refined results indicate that such strategy leads to the modification of the 16c interstitial sites. The electrical performance demonstrates that a modest substitution (x = 0.03) significantly improves both rate performance (113.1 mAh/g, charge and discharge at 5 C) and cycling stability (85% capacity retention after 500 cycles at 1 C). A higher substitution level (x = 0.05) markedly improves high-rate cycling performance, achieving 96% capacity retention after 500 cycles at 5 C. It offers tailored solutions for various application needs, including capacity-focused and high-current-rate applications. Furthermore, the stable LiNi0.5Mg0.05Mn1.45O4 sample could also serve as an effective coating layer for other electrode materials to enhance their cycling stability.

Dual‐Gradient Concentration Distribution in Sb−Cu Alloy Nanoarrays for Robust Sodium‐Ion Storage

AbstractAlloy‐type materials are attractive for anodes in sodium‐ion batteries (SIBs) owing to their high theoretical capacities and overall performance. However, the accumulation of stress/strain during repeated cycling results in electrode pulverization, leading to rapid capacity decay and eventual disintegration, thus hindering their practical applications. Herein, we report a 3D coral‐like Sb−Cu alloy nanoarray with gradient distribution of both elements. The array features a Sb‐rich bottom and a Cu‐rich top with increasing Sb and decreasing Cu concentrations from top to bottom. The former is the active component that provides the high capacity, whereas the latter serves as an inert additive that acts against volume variation. The gradual transition in composition within the electrode introduces a ladder‐type volume expansion effect, facilitating a smooth distribution and effective release of stress, thereby ensuring the wanted mechanical stability and structural integrity. The as‐developed nanoarray affords a high reversible capacity (460 mAh g−1 at 0.5 C), stable cycling (89 % retention over 120 cycles at 1.0 C), and superior rate capability (354 mAh g−1 at 10 C). The concentration dual‐gradient strategy paves a new pathway of designing alloy‐type materials forSIBs.

High-loading NaCrO2 @C nanofibers as binder-free cathode for high-stable sodium-ion batteries

A NaCrO2 @C flexible free-standing cathode is designed and fabricated via a facile electrospinning strategy, in which electrochemically active NaCrO2 nanoparticles homogeneously dispersed in the flexible carbon nanofibers. Serving as the binder-free cathode for sodium-ion batteries, the as-constructed NaCrO2@C flexible free-standing cathode delivers a long cycling life (81 % capacity retention after 1000 cycles) with a high loading (7.6 mg cm−2). The enhancements for sodium-ion insertion/desertion is assigned to the dramatically decrease the polarization between electrodes and avoid the volume expansion during high-rate cycling. The NaCrO2@C flexible free-standing cathode opens up exciting possibilities for the development of advanced flexible sodium-ion batteries with both excellent mechanical flexibility and electrochemical properties.

The high-rate cycling stability of the LiFe0.6Mn0.4PO4/C cathode material is enhanced through in-situ Nb-doping

LiFe0.6Mn0.4PO4/C, due to its low cost and safety advantages, is gradually becoming a safe and reliable commercial lithium battery storage material. However, its lower capacity at high rates and poor cycle performance limit its further industrial application. To address this, this work used a one-step solvothermal method to prepare Li(Fe0.6Mn0.4)1‑xNbxPO4 (x = 0, 0.01, 0.02, 0.03) cathode materials to improve electrochemical performance. Characterization of the samples indicates that Nb doping promoted the growth of the material's [001] crystal orientation, thus enhancing the lithium ion diffusion rate, effectively reducing electrode polarization and charge transfer resistance, which helps to explain its excellent rate performance. More importantly, Nb doping increases the M-O bond energy, making the LMFP/C metal-oxygen framework more stable, and enhancing the stability of the crystal structure of lithium ions intercalating and deintercalating during cycling. The electrochemical test results further indicate that the LFMP/CNb0.02 cathode exhibits excellent electrochemical performance. It has remarkable capacities of 156.9 mAh·g‑1 at 0.2 C and 135.9 mAh·g‑1 at 1 C, particularly showing an initial discharge specific capacity of 121.4 mAh·g‑1 at a high rate of 5 C. After 500 cycles, it still maintains a capacity of 114.3 mAh·g‑1, with a capacity retention rate of 94.15 %, significantly outperforming the original LMFP/C (initial discharge specific capacity of 109.8 mAh·g‑1) which only retains 61.47 % of its capacity after 300 cycles.

Tuning Deposition Conditions for VN Thin Films Electrodes for Microsupercapacitors: Influence of the Thickness

Vanadium nitride is a highly promising material for micro-pseudocapacitors when used as a bifunctional thin film, i.e. an electrode material and a current collector, owing to its remarkable electrical and electrochemical properties. However, the specific limitations associated with high-rate cycling remain unclear. In this study, we evaluate how the characteristic time associated with charge/discharge of vanadium nitride films is modified with the film thicknesses using electrochemical impedance spectroscopy and cyclic voltammetry measurements coupled to a semi-empirical model commonly utilized to assess the high-rate behaviour of battery electrodes. Both methodologies are in good agreement and revealed that rate capability of this bi-functional material is limited by the VN electrical conductivity. To confirm this finding, VN thin films were sputtered on platinum current collectors, leading to a six-fold reduction in the characteristic time associated with charge/discharge of the current collectors/electrode material. This underscores the importance of using current collectors even for highly conductive electrode materials.

Controlling Structure and Morphology of MoS2 via Sulfur Precursor for Optimized Pseudocapacitive Lithium Intercalation Hosts

AbstractMolybdenum disulfide (MoS2)‐based electrode materials can exhibit a pseudocapacitive charge storage mechanism induced by nanosized dimension of the crystalline domains, which is why control over material structure via synthesis conditions is of significance. In this study, we investigate how the use of different sulfide precursors, specifically thiourea (TU), thioacetamide (TAA), and L‐cysteine (LC), during the hydrothermal synthesis of MoS2, affects its physicochemical, and consequently, electrochemical properties. The three materials obtained exhibit distinct morphologies, ranging from micron‐sized architectures (MoS2 TU), to nanosized flakes (MoS2 TAA and LC). While all three synthesized samples exhibit pseudocapacitive Li+ intercalation properties, the capacity retention of the latter two consisting of nanosized flakes is further improved at high cycling rates. The individual charge storage properties are analyzed by operando X‐ray diffraction, dilatometry, and 3D Bode analysis, revealing a correlation between the morphology, porosity, and the electrochemical intercalation behavior of the obtained electrode materials. The results demonstrate a facile strategy to control MoS2 structure and related functionality by choice of hydrothermal synthesis precursors.

Mn2+-Modified Ammonium Vanadate as High Rate and Long Cycle Life Cathode for Aqueous Zinc Ion Batteries

Mn²⁺-Modified Ammonium Vanadate as High Rate and Long Cycle Life Cathode for Aqueous Zinc Ion Batteries

Bimetallic Sulfide Sb2S3/FeS2 Heterostructure Anchored in a Carbon Skeleton for Fast and Stable Sodium Storage.

Sodium-ion batteries (SIBs) are a promising substitute for lithium batteries due to their abundant resources and low cost. Metal sulfides are regarded as highly attractive anode materials due to their superior mechanical stability and high theoretical specific capacity. Guided by the density functional theory (DFT) calculations, 3D porous network shaped Sb2S3/FeS2 composite materials with reduced graphene oxide (rGO) through a simple solvothermal and calcination method, which is predicted to facilitate favorable Na+ ion diffusion, is synthesized. Benefiting from the well-designed structure, the resulting Sb2S3/FeS2 exhibit a remarkable reversible capacity of 536 mAh g-1 after 2000 cycles at a current density of 5 A g-1 and long high-rate cycle life of 3000 cycles at a current density of 30 A g-1 as SIBs anode. In situ and ex situ analyses are carried out to gain further insights into the storage mechanisms and processes of sodium ions in Sb2S3/FeS2@rGO composites. The significantly enhanced sodium storage capacity is attributed to the unique structure and the heterogeneous interface between Sb2S3 and FeS2. This study illustrates that combining rGO with heterogeneous engineering can provide an ideal strategy for the synthesis of new hetero-structured anode materials with outstanding battery performance for SIBs.

Structural Modification Strategy for Enhancing Electrochemical Performance of Electrodes Under High Current Cycling and First Principle Computational Research for Electrode Materials

Recently, there has been significant interest in advancing lithium-ion battery technology due to its widespread use in various applications. Our research delves into this domain, focusing on enhancing the electrochemical properties of batteries through structural modification of electrode materials. Our work demonstrates the significant enhancements of electrochemical performance under high current cycling using structurally modified electrode materials . In first work, crumpled graphene oxide anode proves to be an effective strategy for enhancing its electrochemical properties, attributed to its advantageous crumpled morphology. This morphology allows for improved electrode stability and easier access for lithium ions, enabling them to interact with its larger specific surface area. In second work, we describe enhanced the drawback of reduced electrochemical performance during high-rate cycles by synthesizing multidimensional LFP-based carbon composite. The lithium ion diffusivity and electrode stability of the prepared composite are significantly improved in charging and discharging cycles by introducing graphene quantum dots alongside CNTs, exhibiting superior electrochemical properties even at high current densities. In third work, density functional theory simulation is employed for demonstrating the enhanced electrochemical properties of prepared electrodes by exploring their properties. Our research provides insights into electrode material design as an effective approach to enhancing the electrochemical properties of lithium-ion batteries.Acknowledgement:This work was supported by the National Research Foundation of Korea (NRF-2021R1A2C1008272). This work was supported by Ministry of Trade, Industry and Energy, KEIT, under the project title"International standard development of evaluation methods for nano-carbon-based high-performance supercapacitors for electric vehicles" (project # 20016144).

Synergy of Silicon-Graphene Anodes and Polymer-Ceramic Hybrid Separators for High Rate-Capable Lithium-Ion Batteries

With more and more electric vehicles (EV) hitting the market, the need for better and more robust energy storage system increases, and silicon has been a promising candidate for the next generation anode material to satisfy the high energy density and high-power requirements for electric vehicles because of its extremely high theoretical capacity. This has allowed the design of thinner electrodes to reduce the diffusion time scales and deliver a fast charge. However, at high charge and discharge rates, low electrical conductivity (~1.12 eV) of silicon hampers the battery performance. As a result, a lot of research has been conducted to improve the performance of silicon anodes using nanoscale carbon to increase the electrical conductivity. Graphene has been used to synthesize Si/Gr hybrid anodes due to its high conductivity.Graphene nanoribbons (GNRs) , a part of the graphene family, are one-dimensional graphene nanostructures which tune its electrical properties based on dimensional confinement. GNR has a higher conductivity than Graphene. It also has high aspect ratio and surface area to provide a strong conductive path along with mechanical strength to support the silicon anode. Due to presence of GNR, lithium-ion transport into silicon nanostructures was enhanced. As a result, 50% of graphene was replaced by 50% GNR with silicon nanoparticles to form anodes. Due to the highly conducting structure of GNR, capacity at high rates was significantly improved because of the improved silicon utilization. Since GNR’s dimensions are in nanometer range, connection with silicon nanoparticles is better. It not only improves silicon to silicon conductivity, but it also acts as a filler for better connection of graphene with silicon nanoparticles.Addition of graphene nanoribbons can improve the lithium-ion transport within the anode but to enhance the high charge transfer rate further, Si/GNR/Gr hybrid, high rate-capable anodes were paired with Polyimide (PI)/Polysilsesquioxane (PSSQ) hybrid separators which also shown to exhibit an improved charge transfer rate. At high rates such as 3C and 5C, the effect of separator on the cell performance becomes more prominent. While Celgard’s performance was very unstable at both 3C and 5C, at 3C, the cycling of hybrid separators did not get impacted, despite the relatively harsher conditions. This synergistic combination of high-rate capable silicon/graphene anode and hybrid separator outperformed the commercially used separator especially at high-rate cycling. Cells with Si/GNR/Gr anode paired with the PI/PSSQ separator delivered an impressive capacity of 1,000 mAh/g at high charge/discharge rates of 5C/5C.

One-Pot Aqueous Spray Drying of Hierarchical Na3V2(PO4)3 (NVP) Particles for High-Performance Sodium-Ion Batteries

Sodium-ion batteries (NIBs) have been recognized as a promising alternative to lithium-ion batteries (LIBs), especially for stationary large-scale applications that favor inexpensive storage over high energy density, as their cathode materials don’t require scarce and expensive elements such as Li, Co, and Ni.1,2 Na3V2(PO4)3 (NVP) offers high ionic conductivity and long term stability due to its sodium super ionic conductor (NASICON) structure3. However, it suffers from poor electronic conductivity and requires energy-intensive synthesis routes4. Spray drying has recently become a common energy-effective route but requires organic solvents5 or complex carbon additives6. In this study, a more efficient and sustainable aqueous spray-drying method is presented to synthesize carbon-coated NVP by using L-ascorbic acid as a carbon source. Additionally, the role of conductive additives is explored in low-carbon samples. NVP sodium-ion half cells showed very high reversible capacity (114.7 mAh g-1 at 0.2C), high rate capability (80.8% capacity retention at 30C), and long cycling performance (93.8% capacity retention after 5000 cycles at 10C). The exceptional cycle life makes it a promising candidate for grid level energy storage. Furthermore, if configured without an intercalation anode material, the "host-free" NVP cells hold the promise to substitute the widely used LiFePO4 batteries for EV applications7. References (1) Liu, J. Addressing the Grand Challenges in Energy Storage. Advanced Functional Materials. February 25, 2013, pp 924–928. https://doi.org/10.1002/adfm.201203058.(2) Schneider, S. F.; Bauer, C.; Novák, P.; Berg, E. J. A Modeling Framework to Assess Specific Energy, Costs and Environmental Impacts of Li-Ion and Na-Ion Batteries. Sustain Energy Fuels 2019, 3 (11), 3061–3070. https://doi.org/10.1039/c9se00427k.(3) Zhang, X.; Rui, X.; Chen, D.; Tan, H.; Yang, D.; Huang, S.; Yu, Y. Na 3 V 2 (PO 4 ) 3 : An Advanced Cathode for Sodium-Ion Batteries. Nanoscale. Royal Society of Chemistry February 14, 2019, pp 2556–2576. https://doi.org/10.1039/c8nr09391a.(4) Tang, X.; Ding, H.; Teng, J.; Zhao, H.; Li, J.; Zhang, K. Green and Scalable Synthesis of Na3V2(PO4)3 Cathode and the Study on the Failure Mechanism of Sodium-Ion Batteries. ACS Appl Energy Mater 2023, 6 (16), 8443–8454. https://doi.org/10.1021/acsaem.3c01195.(5) Pi, Y.; Gan, Z.; Li, Z.; Ruan, Y.; Pei, C.; Yu, H.; Han, K.; Ge, Y.; An, Q.; Mai, L. Methanol-Derived High-Performance Na3V2(PO4)3/C: From Kilogram-Scale Synthesis to Pouch Cell Safety Detection. Nanoscale 2020, 12 (41), 21165–21171. https://doi.org/10.1039/d0nr04884d.(6) Zhang, J.; Fang, Y.; Xiao, L.; Qian, J.; Cao, Y.; Ai, X.; Yang, H. Graphene-Scaffolded Na3V2(PO4)3 Microsphere Cathode with High Rate Capability and Cycling Stability for Sodium Ion Batteries. ACS Appl Mater Interfaces 2017, 9 (8), 7177–7184. https://doi.org/10.1021/acsami.6b16000.(7) Ma, B.; Lee, Y.; Bai, P. Dynamic Interfacial Stability Confirmed by Microscopic Optical Operando Experiments Enables High-Retention-Rate Anode-Free Na Metal Full Cells. Advanced Science 2021, 8 (12). https://doi.org/10.1002/advs.202005006. Figure 1

Elucidating the Electrochemical Impact of the Calendering Process on Three-Dimensional Designed Electrodes for Lithium-Ion Batteries

Significant advancements in battery technology are imperative to meet the ambitious demands for electromobility and stand-alone energy storage devices. This stems from the need to achieve operations with high energy and power density, coupled with stringent safety standards and extended lifespans, while reducing production and material costs. The preferred energy storage technology for the coming decade is anticipated to remain lithium-ion battery (LIB) technology. The focus on researching high-energy active materials to optimize this technology is paramount. In addition to optimizing materials, significant performance enhancements can be achieved by using electrodes with high mass loading and a multiscale tailored electrode design that can be scaled up to production level.The technological challenges of achieving a breakthrough in gaining simultaneously high energy and power density characteristics while maintaining high process and operational reliability with significant cost savings are the subject of current research and development in the field of LIB technology. To tackle this, the study explores the laser-assisted generation of three-dimensional (3D) electrode architectures and assesses its impact on battery performance and future integration into battery production. The advanced electrode design involves micro and sub-micron structures that can be tailored in various ways, leading to notable improvements in battery lifespan, battery safety, and fast charging and high-power operation capabilities compared to batteries with conventional two-dimensional (2D) electrodes. High-power ultrafast laser ablation emerges as a precise method for introducing such structures.Coordinating the production of 3D electrodes with laser assistance necessitates synchronization with established manufacturing steps in the battery production process. Notably, the calendering of electrodes holds significance due to its substantial influence on the microstructural properties of the electrode material, encompassing porosity, material density, and layer adhesion. The study investigates the impact of laser-induced structuring, encompassing micro-/nano-porosities and microtopography, on electrodes with varying mass loadings ranging from 2mAh/cm² to 6mAh/cm². Electrochemical characteristics such as high-rate capability, fast charging, and cycle lifetime are evaluated accordingly, employing cells with graphite anodes and lithium-nickel-manganese-cobalt oxide cathodes.