High-energy Lithium-ion Batteries Research Articles

Scalable Direct Recycling of Cathode Black Mass from Spent Lithium‐Ion Batteries

AbstractEnd of life (EoL) lithium‐ion batteries (LIBs) are piling up at an intimidating rate, which is alarming for environmental health. With further expected rapid growth of LIB use, the magnitude of spent battery accumulation is also expected to grow. LiNixCoyMnzO2 (NCM) cathode materials are a dominant chemistry in high energy LIBs, and make up a huge portion of this waste accumulation. Direct recycling is one of the most promising ways to turn this waste to wealth, but has been limited to lab‐scale, due to lack of robustness, namely the tedious pretreatment required that involves toxic organic solvents. Herein, a process that integrates the pretreatment and relithiation of the cathode black mass is demonstrated. Cathode material from EoL electric vehicle (EV) batteries is treated in a 100 g per batch operation and the regenerated cathode active material demonstrates 100% electrochemical performance recovery, with 91% yield rate, and shows promise for further scale up. This process has the advantages of integration, scalability, and universality, which clears the barricade for direct recycling to move from lab to industry scale with considerable profitability.

A scalable silicon/graphite anode with high silicon content for high-energy lithium-ion batteries

High-capacity Si-based anodes are urgently needed for high-energy lithium-ion batteries in forthcoming electric vehicles and energy storage systems. However, it is still a challenge to prepare Si anodes with high Si content materials as well as good electrochemical performance because the accumulation and growth of Si lead to large volume expansion, pulverization and cycling degradation. Herein, we demonstrate feasibility of a high-capacity Si-based anode via a scalable and simple route using high Si content (31.6 wt%) Si/graphite composite, consisting of thin Si nanolayer and edge-sites-exposed graphite. This architecture effectively alleviates the volume changes of Si and facilitates lithium-ion transport. As a result, the Si/graphite composite delivers a reversible capacity of 1,080 mAh/g with an initial Coulombic efficiency of 86.3% and achieves outstanding cycling stability (94.3% capacity retention after 100 cycles). When combined with commercial graphite-blended systems for a 1.5 Ah pouch-type full-cell test under a high electrode density (1.6 g/cm3) and areal capacity (3.46 mAh/cm2), the composite demonstrates excellent cycling stability at 25 and 45 °C, respectively, and good high-rate performance. This strategy offers a practical feasibility of next-generation high-capacity anode for high-energy LIBs.

Atomic Horizons Interpretation on Enhancing Electrochemical Performance of Ni-Rich NCM Cathode via W Doping: Dual Improvements in Electronic and Ionic Conductivities from DFT Calculations and Experimental Confirmation.

The rapid capacity degradation and poor rate capability hinder the application of Rich-Ni layered LiNix Coy Mnz O2 (NCM) as cathode materials for high-energy lithium-ion batteries. In this study, density functional theory (DFT) calculations, combined with conventional electrochemical measurements, reveal from the atomic view that the dual improvements in electronic and ionic conductivities are the main facts for the property enhancement. The bandgap of the cathode material is reduced to 1.1623eV due to the increased number of electrons near the Fermi level after W intercalation. Such improved electronic conductivity subsequently leads to a suppressed polarization and reduced resistance, enabling an improved cycle life of up to 93.97% after 100 cycles at 0.5 C. Furthermore, the doping with W6+ also introduced a strong WO bond into the layered structure so that the thickness of the Li slab is expanded to 2.6476 Å, which reduces the energy barrier from 0.355 to 0.308eV for the migration of Li+ within the Li slab, as confirmed by the DFT calculation. Consequently, the rate performance is greatly improved due to the reduced diffusion energy, with a specific capacity of 159.11 mAg-1 even at 5 C rate, indicating high potential for future applications.

In situ mitigating cation mixing of Ni-rich cathode at high voltage via Li2MnO3 injection

Ni-rich layered oxides (LiNixCoyMnzO2, x ≥ 0.8) have been under intense investigation as cathode materials for high-energy rechargeable lithium ion batteries (LIBs) due to their high capacity and relatively low cost. However, Ni/Li cation mixing, in most cases, brings about capacity degradation, structure evolution and poor thermal stability, especially at high cut-off voltage. Herein, a universal strategy with novel mechanism-in situ mitigating cation mixing at 4.55 V via injecting Li2MnO3 has been achieved (label as LD-NCM811), significantly improving the electrochemical property, structural integrity and thermal stability of Ni-rich cathode materials compared with the conventional NCM811. LD-NCM811 maintains a high capacity retention of 93% at 0.3 C after 200 cycles at 25 °C with negligible voltage decay of 40 mV, whereas the NCM811 shows a retention of 68% and large voltage decay of 248 mV, and the corresponding cation mixing has been mitigated from 13.5% to 7.5%. At the temperature of 45 °C, LD-NCM811 still keeps a considerable capacity retention of 93% at 1 C, significantly superior to the NCM811 with 75%. Characterization and calculation reveal that the excellent performances result from the Li2MnO3 phase with unique superlattice providing lithium voids in transition metal (TM) oxide layers when it is charged above 4.5 V, which is favorable for the mixed Ni ions migrating back to TM layers instead of blocking the lithium channel. This new finding establishes a general strategy for mitigating cation mixing of NCM811 to realize its application in high energy density and safety batteries.

Ultrahigh areal capacity silicon anodes realized via manipulating electrode structure

High areal capacity is critical towards the practical application of silicon anodes for high-energy lithium ion batteries. Herein, a free-standing silicon-graphene (3D-Si/G) anode with ultrahigh areal capacity is proposed by manipulating electrode structure using 3D-printing. For the 3D-Si/G electrodes with the circle-grid pattern, electrode thickness and printed filament spacing can be precisely constructed and adjusted by controlling a computer program. In this configuration, the tailored free space between and inside the filaments are enough to withstand volume fluctuation of silicon anodes, which significantly improves the structure stability and integrity of electrodes and endows the great accessibility to lithium ions transport in thick electrodes. Furthermore, the unique edge-coaxial and internal-disordered structure in printed filaments greatly enhances the electrode mechanical stability. Simultaneously, the graphene framework with excellent electron-ion transport characteristic ensures fast electrochemical reaction kinetics and low electrochemical polarization in thick electrodes. Therefore, the optimized 3D-Si/G electrode achieves a favorable cycle stability with 8.5 mAh cm −2 after 70 cycles (capacity retention of 75.4%). And the 3D-Si/G thick electrode with four layers achieves a reversible ultrahigh areal capacity of 16.2 mAh cm −2 . More importantly, the easy ink preparation and controllable printing process provide broad prospects for the commercial application of silicon anodes.

The pursuit of commercial silicon-based microparticle anodes for advanced lithium-ion batteries: A review

Silicon (Si) is one of the most promising anode materials for high-energy lithium-ion batteries. However, the widespread application of Si-based anodes is inhibited by large volume change, unstable solid electrolyte interphase, and poor electrical conductivity. During the past decade, significant efforts have been made to overcome these major challenges toward industrial applications. This review summarizes the recent development of microscale Si-based electrodes fabricated by Si microparticles or other industrial bulk materials from the perspective of industrialization. First, the challenges for microscale Si anodes are clarified. Second, structural design strategies of stable micro-sized Si materials are discussed. Third, other critical practical metrics, such as robust binder construction and electrolyte design, are also highlighted. Finally, future trends and perspectives on the commercialization of Si-based anodes are provided.

Investigation on high-energy Si anode mechanical-electrochemical-thermal characteristic under wide temperature range

Studying the cyclic evolution of high-energy Si anode, including the mechanical deformation, voltage hysteresis, heat generation and temperature response, is of great significance for its performance and safety. In this paper, a novel coupled semi-analytical model is developed to investigate the mechanical-electrochemical-thermal characteristic of Si particle anode. This model is adopted a series of temperature and concentration dependent parameters related to electrochemical reaction and Li+ diffusion. The results show that Li+ diffusion process will be limited at a lower initial temperature, which may increase the elastic–plastic stress. Thus, the stress-induced voltage hysteresis is more evident, resulting in the capacity loss and polarization heat increase. In the aspect of thermal behavior, the heat generation during lithiation is more than that during delithiation at each initial temperature, and the total heat accumulation after one cycle is greater at a higher initial temperature. Besides, the asymmetrical elastic–plastic deformation and heat accumulation during cyclic lithiation/delithiation may lead to ratcheting deformation of the Si particle electrode. The ratcheting deformation will be aggravated at a lower temperature. Additionally, the effects of charging rates (0.2C, 0.5C and 1C) are also discussed. The increased charging rate leads to a steeper concentration gradient, the more obvious asymmetrical elastic–plastic deformation, and earlier reaching the cut-off voltage. The electrode will produce more heat in a short time in the case of fast charging, and the resulting self-heating accumulation will affect its thermal stability. Based on this, ratcheting deformation at a fast charging rate is more severe, which will further decrease the mechanical stability of the Si electrode. The theoretical results are verified by the experiments. This study provides a theoretical and experimental basis for understanding the comprehensive performance of high-energy lithium-ion batteries, as well as design and management guidance.

Ta Doping Improves the Cyclability and Rate Performance of a Nickel-Rich NCA Cathode via Promoted Electronic and Cationic Conductivity

NCA layered cathode materials are characterized by low cost and high reversible specific capacity compared with olivine and spinel cathodes. However, the high Ni content also leads to poor cyclability. In this paper, other than the mechanism reported by another group, we proposed the increase in electronic and cationic conductivity of Ta-doped LiNi0.94Co0.04Al0.02O2 cathode material could be the other reason for the promoted electrochemical behavior. DFT calculation revealed that the increased amount of electrons near Fermi energy which reduces the bandgap (from 1.2953 eV to 1.2171 eV) of Ta-NCA can be ascribed to the enhanced electronic conductivity. Such improvement later leads to reduced polarization and therefore the cyclability of the half cell is increased. Meanwhile, the suppressed H2–H3 phase transition, is also found to be responsible for the promoted cyclic performance. For the Ta-NCA cathode, the capacity retention after 100 cycles is promoted from 42.11% to 93.62% (from 81.16 mAh·g–1 to 181.54 mAh·g–1). Ta doping also increases the Li diffusion coefficient due to the expanded interplanar spacing of the Li slab. For Ta-NCA cathode with a promoted diffusion coefficient of 3.11 × 10–11 cm2·s–1, the specific capacity at 5C is increased from 118.51 mAh·g–1 to 158.47 mAh·g–1. Both the increase in cyclability and rate behavior indicate the high potential of the Ta-NCA cathode material in high-energy lithium-ion batteries.

Unraveling the degradation mechanism of LiNi0.8Co0.1Mn0.1O2 at the high cut-off voltage for lithium ion batteries

LiNi0.8Co0.1Mn0.1O2 (NCM811) layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries (LIBs) due to high discharge capacities and energy densities at high operation voltage. However, the capacity fading under high operation voltage still restricts the practical application. Herein, thecapacity degradationmechanismof NCM811 at atomic-scale isstudied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy (STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V, which is distinguished from the generally accepted structure evolution of layered, disordered layered, defect rock salt and rock salt phases, also observed under 4.3 and 4.7 V. The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk, not the previously reported only Li/Ni interlayer mixing. The degradation mechanism of NCM811 at a high cut-off voltage of 4.9 V is attributed to the formation of intergranular cracks induced by defects, the direct formation of the rock salt phase, and the accompanied reduction of Ni2+ and Co2+ phases from the surface to the bulk.

Mo2C catalyzed low-voltage prelithiation using nano-Li2C2O4 for high-energy lithium-ion batteries

Irreversible lithium loss in the initial cycles appreciably reduces the energy density of lithium-ion batteries. Prelithiation is an effective way to compensate for such lithium loss, but current methods suffer from either the instability or low capacity of prelithiation reagents. Lithium oxalate (Li2C2O4) has shown great potential as a lithium-compensation material because of its high theoretical capacity (equivalent to lithium metal), low cost, and air stability. However, the practical applications of Li2C2O4 are limited by its low electrochemical activity and high critical decomposition voltage. In this study, we performed the prelithiation of a low-voltage cathode by using Mo2C catalysis and nano-Li2C2O4. Results show that the Mo2C catalyst changes the electron cloud distribution around Li2C2O4 and greatly reduces the activation energy, thereby significantly accelerating the lithium release from Li2C2O4. The nano-Li2C2O4 prepared by freeze-drying shows accelerated ionic and electronic conduction as well as close contact with Mo2C. Benefiting from the synergistic effect, the decomposition potential of Li2C2O4 is decreased by 0.5 V with an efficiency close to 100%. The LiCoO2∥SiO full cell empowered with the nano-Li2C2O4/Mo2C prelithiation composite demonstrates 46.9% higher capacity than the control and thus has great potential for practical applications.

Flexible and ultralight MXene paper as a current collector for microsized porous silicon anode in high-energy lithium-ion batteries

Silicon (Si) is a new candidate anode material for lithium-ion batteries. The porous treatment of Si anode has been proved to be effective. In order to improve the interface performance and energy density of batteries, we start from the current collector (CC) and make further improvements. Combined with the advantages of new two-dimensional material MXene in electrochemical aspects, we make MXene replace the traditional Cu foil as CC of Si anode. The prepared MXene paper is both flexible and lightweight. After coating the Si slurry on it, the assembled half cells and 5 V-class full cells can achieve normal lithium-ion intercalation and deintercalation. Moreover, compared with the battery using Cu current collector, the volume expansion of porous silicon in the battery with MXene is further alleviated, and the cycle stability performance is also improved.

Stabilizing structure and voltage decay of lithium-rich cathode materials

A major challenge in the discovery of high-energy lithium-ion batteries (LIBs) is to control the voltage stability and Li+ kinetics in lithium-rich layered oxide (LrLO) cathode materials. Although these materials can provide a higher specific capacity compared to the current industrially used cathodes, the substantial voltage decay and low Li+ diffusion during long term cycling is a serious reason for hindering their practical applications. In order to suppress the voltage decay in lithium-rich cathode materials, herein we introduce the Ti doping into Li1.2Mn0.56Ni0.17Co0.07O2 cathodes. Also, the influence of Ti doping on the crystalline internal structure, surface chemistry, cycling retention, and Li+ kinetics of Li1.2Mn0.56Ni0.17Co0.07O2 cathodes have been focused in this work. The Ti doping effectively enhances the structural/interfacial stability of the cathode and accelerates the Li+ kinetics by expanding the lattice, thereby significantly realizing its voltage/cycling stability and high-rate capability. Experimental results show that Ti-doped LrLO (1% Ti) has achieved high electrochemical kinetics as the discharge cycle retention increased from 61.58% (pristine) to 80.0% after 180 cycles at 1 C, with 150.3 mAh g−1 showing superior high-rate performance at 5C. Ex-situ XRD results confirmed the better structural stability of Ti-doped LrLO after high-rate electrochemical cycling. Our findings provide a suitable element doping strategy for regulating the voltage decay and cycle retention of LrLO, thus promoting their real-world application in future batteries.

Rapid Self-Healing Gel Electrolyte Based on Deep Eutectic Solvents for Solid-State Lithium Batteries.

A deep eutectic solvent (DES) is a promising electrolyte choice for lithium metal batteries. However, the DES liquid electrolyte causes safety concerns and side reactions with the lithium anode. Therefore, it is necessary to solidify the DES-based electrolyte and enhance its electrochemical stability. Herein, we present a novel DES-based rapid self-healing gel electrolyte, which is able to self-smooth its surface cracks in only 30 min. The electrolyte exhibits noncombustibility (SET = 4 s g-1), high ionic conductivity (1.1 × 10-3 S cm-1 at 25 °C), and a wide electrochemical voltage window (4.5 V vs Li/Li+). As a result, the solid-state lithium batteries coupling the gel electrolyte with the Li anode and LiFePO4 cathode deliver a high specific capacity of 135.4 mA h g-1 with durable cyclic stability (>1200 h). This work provides valuable insights for design of fire-resistant and high-energy solid-state lithium batteries.

Towards fast-charging high-energy lithium-ion batteries: From nano- to micro-structuring perspectives

Electric vehicles (EVs) have been playing an indispensable role in reducing greenhouse gas emissions for our modern society. However, current EVs are difficult to meet people’s diverse travel needs, especially in long endurance and fast-charging capacities. At the heart of this issue is the physicochemical limit of current lithium-ion batteries (LIBs), which are the core parts for powering the vehicles. Hence, LIBs with simultaneous high energy and power are critically required to further promote the development of EVs. In this review, we first summarize the key electrochemical processes in electrochemical reactions which lead to the corresponding overpotentials in or between multiple battery components. Furthermore, numerical simulations are employed to quantitatively analyze the effects of versatile electrode parameters on electrochemical properties in high-energy NMC811//graphite systems. On the basis of the in-depth understandings from simulation, recent experimental efforts on designing electroactive materials and electrode architectures across multiple length scales are discussed. Among them, nano-structuring can promote local mass transport and stabilize the interfaces at the particle level, while micro-structuring can establish efficient pathways for charge carriers at the electrode level. Finally, we conclude that a tight feedback loop among structure engineering, characterization and simulation should be followed to speed up the understanding of the deficiencies existing in current electrode designs as well as point out the possible electrode optimization routes for next-generation fast-charging LIBs.

Synergistic Effect of Bis(2,2,2-trifluoroethyl) Carbonate and Succinonitrile in Suppressing the Dissolution of Nickel for Performance Improvement of Nickel-Rich Lithium Metal Batteries

Nickel-rich layered transition metal (TM) oxide cathode materials become the prospective candidates for high-energy lithium-ion batteries on account of their significant role in improving specific energy and power density. However, the decomposition of the electrolyte caused by the catalytic reaction of highly active Ni4+ ions together with the deposition of TM ions dissolved into the electrolyte upon the anode surface eventually deteriorates the capacity and cycling stability of nickel-rich lithium metal batteries. Herein, the effectively synergistic effect of a bis(2,2,2-trifluoroethyl) carbonate (BTFC) and succinonitrile (SN) electrolyte in suppressing the TM nickel ion dissolution in a nickel-rich lithium metal battery by building a reliable and protective electrode/electrolyte interface was reported. While SN was used to improve the electrochemical stability of the electrolyte, the oxidation products of BTFC can form a dense and stable passivated layer covering up the surface of the electrode. With the strong coordination ability of F bonding to the high-valence Ni ions, the continued TM nickel ion dissolution in the hybrid electrolyte was prevented. Thus, the NCA||Li cell with the designed electrolyte demonstrates an obvious improvement of capacity retention from 53.3% to 82.1% after 100 cycles compared with a conventional electrolyte. The remarkable rate performance is witnessed with high specific capacity over 120 mAh g–1 at the rate of 1000 mA g–1. The results provide insight into improving the performance of Ni-rich lithium metal batteries by the electrolyte manipulation strategy. The fundamental mechanism understanding of this synergistic effect in this study may facilitate the development of cooperative electrolytes with an advanced nickel-rich cathode for next-generation batteries.

High-Energy Metallic Lithium Batteries Enabled by Polymer-in-Salt Electrolytes of Cyclic Carbonate Substituted Polyethers

High-Energy Metallic Lithium Batteries Enabled by Polymer-in-Salt Electrolytes of Cyclic Carbonate Substituted Polyethers

One-Step Synthesis of LiCo1-1.5xYxPO4@C Cathode Material for High-Energy Lithium-ion Batteries.

Intrinsically low ion conductivity and unstable cathode electrolyte interface are two important factors affecting the performances of LiCoPO4 cathode material. Herein, a series of LiCo1-1.5xYxPO4@C (x = 0, 0.01, 0.02, 0.03) cathode material is synthesized by a one-step method. The influence of Y substitution amount is optimized and discussed. The structure and morphology of LiCo1-1.5xYxPO4@C cathode material does not lead to obvious changes with Y substitution. However, the Li/Co antisite defect is minimized and the ionic and electronic conductivities of LiCo1-1.5xYxPO4@C cathode material are enhanced by Y substitution. The LiCo0.97Y0.02PO4@C cathode delivers a discharge capacity of 148 mAh g−1 at 0.1 C and 96 mAh g−1 at 1 C, with a capacity retention of 75% after 80 cycles at 0.1 C. Its good electrochemical performances are attributed to the following factors. (1) The uniform 5 nm carbon layer stabilizes the interface and suppresses the side reactions with the electrolyte. (2) With Y substitution, the Li/Co antisite defect is decreased and the electronic and ionic conductivity are also improved. In conclusion, our work reveals the effects of aliovalent substitution and carbon coating in LiCo1-1.5xYxPO4@C electrodes to improve their electrochemical performances, and provides a method for the further development of high voltage cathode material for high-energy lithium-ion batteries.

Size controllable single-crystalline Ni-rich cathodes for high-energy lithium-ion batteries.

A single-crystalline Ni-rich (SCNR) cathode with a large particle size can achieve higher energy density, and is safer, than polycrystalline counterparts. However, synthesizing large SCNR cathodes (>5μm) without compromising electrochemical performance is very challenging due to the incompatibility between Ni-rich cathodes and high temperature calcination. Herein, we introduce Vegard's Slope as a guide for rationally selecting sintering aids, and we successfully synthesize size-controlled SCNR cathodes, the largest of which can be up to 10μm. Comprehensive theoretical calculation and experimental characterization show that sintering aids continuously migrate to the particle surface, suppress sublattice oxygen release and reduce the surface energy of the typically exposed facets, which promotes grain boundary migration and elevates calcination critical temperature. The dense SCNR cathodes, fabricated by packing of different-sized SCNR cathode particles, achieve a highest electrode press density of 3.9g cm-3 and a highest volumetric energy density of 3000Wh L-1. The pouch cell demonstrates a high energy density of 303Wh kg-1, 730Wh L-1 and 76% capacity retention after 1200 cycles. SCNR cathodes with an optimized particle size distribution can meet the requirements for both electric vehicles and portable devices. Furthermore, the principle for controlling the growth of SCNR particles can be widely applied when synthesizing other materials for Li-ion, Na-ion and K-ion batteries.

(Battery Division Technology Award) Understanding Metals' Roles in Layered Structure Oxides for High-Energy Lithium-ion Batteries

The ever-increasing requirements in the high-energy density of lithium-ion batteries (LIBs) and current bottlenecks in cobalt supply place restrictions on the development of the state-of-the-art cathode materials with fine-tuned chemical composition by substituting the cobalt with nickel and manganese. In the layered structure ternary systems (LiNi1-y-zMnyCozO2, NCM), three transition-metal ions play a distinctive role that determines the physicochemical properties. A comprehensive understanding of the basic contribution of each transition metal is critical for further complete replacing expensive cobalt.[1] Here, we demonstrate cobalt and manganese behaviors by comparing various layered oxides with different chemical compositions to reveal their corresponding contributions.[2] Our results affirmed that cobalt plays an undeniable role in fast degradation, and found that cobalt is more destructive than Ni at high voltages. Even the possible instability induced by manganese (III) Jahn-Teller distortion [3], Mn(IV) substitution in the lattice can effectively alleviate this destructive and enables a high potential functionality. By further regulating the chemical composition with a concentration gradient strategy, Co-enriched surface and Mn-enriched core design in Ni-rich particles determines a robust structure, which can effectively suppress the owing to the low stiffness of the surface and stable structure in the core region. With these fundamental discoveries, we provide a guide for developing the promising Co-free cathodes to meet the increasing demand for high-energy density LIBs.

(Invited) 3D Electrode Architectures for High Power and High Energy Lithium-Ion Battery Operation - Recent Approaches and Process Upscaling

During the next decades, combustion driven cars will be completely replaced by electrical vehicles (EVs) and it seems quite obvious that liquid electrolyte lithium-ion batteries (LIBs) will be the dominating energy storage system for the next at least 5 to 10 years. As a consequence, in Europe numerous Gigafactories have recently been planned with this state of technology. However, the current lithium-ion battery technology suffers so far from some restrictions like the inability to combine high power and high energy operations at the same time. This limitation is mainly attributed to the cathode architecture and respective mass loading. In addition, the further demand for a significantly enhanced fast charging mainly requires an optimization of the anode design flanked by a high areal capacity. Advanced 3D electrode architectures based on a thick film electrode concept seem to be the most promising approach to overcome the current limitations in battery performances. However, respective technology innovations need to provide a high compatibility grade to existing manufacturing routes in order to enable the required integration in existing and planned factories. For so-called “generation 3” materials, i.e., nickel-rich lithium nickel manganese cobalt oxide (NMC) cathode and silicon-based anode materials, structuring technologies using cutting edge ultrafast high power lasers, are being developed in order to manufacture 3D electrode architectures with high areal capacity. Multibeam laser processing using diffractive optical elements and dual scanner approaches were established in order to enable high processing speeds in roll-to-roll electrode handling systems. The technology readiness level (TRL 6) is demonstrated for pouch cells geometries. For water-based NMC 622 and silicon-graphite composites the laser structuring process was developed. Different structures including hole, grid, and line patterns, were studied regarding their impact on electrochemical performances such as high-rate capability and cell lifetime. Lithium concentration profiles of unstructured and structured electrodes were studied post mortem using laser-induced breakdown spectroscopy (LIBS) in order to evaluate lithium intercalation/deintercalation efficiencies and detect possible cell degradation processes. In comparison to unstructured electrodes, 3D electrodes could hereby always be identified as superior: unstructured thick film electrodes show a significant drop in capacity retention for high power operation and tend to form hot spots acting as starting point for cell failure. The upscaling process is flanked by a further improvement of electrode design. For this purpose very recently laser induced forward transfer (LIFT) is applied as printing technology to draw new concepts for sophisticated model electrode architectures with advanced electrochemical performances. Finally, the micro-/nano-scaled texturing of current collectors and separator material is discussed as further possible approaches for boosting the electrochemical performances of LIB pouch cells.