Li-air Research Articles

Adapting Single-Atom Catalysts to Li-O2 Batteries: Enhancing Energy Storage.

Lithium-oxygen (Li-O₂) batteries (LOBs) are promising candidates for energy storage, primarily due to their remarkable energy density. Yet, the practical implementation of LOBs is hampered by the large overpotentials they require during charging, given the Li₂O₂ they produce is not conductive. This both undermines their energy efficiency and accelerates associated solvent breakdown. Enhancing oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics at cathodes is essential to mitigating these issues, as elevating corresponding activity reduces charge polarization and prolongs battery lifespan, addressing challenges impeding current LOB adaptation. Recently, single-atom catalysts (SACs) garnered interest from LOB researchers for their exceptional catalytic activity, stemming from their maximized surface exposure and related properties. This review first examines SAC structural design and morphological features that contribute to catalytic behavior, then illustrates how theoretical approaches such as density functional theory uncover mechanistic pathways driving SAC performance. This analysis encompasses preferred atomic arrangements, adsorption behaviors, active site charges, and electronic structure modifications relevant to LOBs. Subsequently, this review investigates how SACs influence catalytic efficiency, highlighting their practical value in advancing LOB technology. Last, current obstacles are summarized and prospects of SAC synthesis, analysis, and implementation are discussed, offering insights toward future research directions.

Ni/Co Dual Atom Catalysts with Synergistic Bifunctionality for High-efficiency Lithium Oxygen Battery

Ni/Co Dual Atom Catalysts with Synergistic Bifunctionality for High-efficiency Lithium Oxygen Battery

Machine Learning-based Battery Life Detection and Photoelectrode Materials Selection for Lithium Batteries

Abstract Herein, we developed three-dimensional pristine titanium dioxide (TiO2) photo-electrocatalyst material (PEM) with homogeneous distribution of oxygen vacancies (OV) for lithium-oxygen (Li-O2) battery system (denoted as LOBs) under illumination. This rationally designed OV-TiO2 photoelectrode-catalyst has exhibited excellent capacity, small overpotential, long-term cycle stability, and higher rate capability performance according to our electrochemical experiment study. In short, OV as photoinduced charge separation centers (inert surface atomic modification method) fascinate the effective separation of electrons (e−) and holes (h+). In turn, induced e− and h+ are beneficial to the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) process. More importantly, machine learning (ML) algorithms to analyze and optimize battery performance are innovative in the photoelectrical field. The utility of ML analysis is extensively shown to be effective in learning the in/output connection of interest. Based on ML analysis results, the OV-TiO2 cathode is indeed the key point to extend the LOB life span. More importantly, our brilliant anatase OV-TiO2 revealed the optimization of electrode material for high performance and reversibility in LOBs. We expect that it will bring special OV-TiO2 and some other hierarchical hollow nanomaterials, a big step toward battery technology no matter in cost-effectiveness and environmentally friendly aspects.

S-decorated Mo2C as efficient catalyst for Li-O2 battery system.

Lithium-oxygen (Li-O2) batteries are considered an important candidate for the next generation of energy storage systems due to their ultra-high theoretical energy density (11 586 mA h g-1), but their slow kinetic reactions, high overpotential and cyclic instability seriously limit their practical applications. In this study, sulfur modified Mo2C (S@Mo2C) cathode materials were prepared by hydrothermal synthesis by sulfur (S) doping to optimize the electronic structure and catalytic activity of Mo2C (Mo2C). Experiments show that S@Mo2C exhibits significantly improved electrochemical performance compared to commercial Mo2C: its specific capacity is up to 3955 mA h g-1 (commercial material only 508 mA h g-1), the charge and discharge overpotential is reduced to 0.26 V (53.6%), and the capacity retention rate remains 77.8% after 250 cycles. X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analysis showed that the introduction of sulfur induced the formation of a heterostructure of MoS2/MoS3 in the Mo2C lattice, which enhanced the conductivity and oxygen reduction/precipitation (ORR/OER) activity of the material. In addition, sulfur doping promotes the formation of highly conductive amorphous Li2O2 and effectively inhibits the accumulation of insulating ring Li2O2, thus significantly improving the cycle stability and energy efficiency of the battery. This study provides a new structural regulation strategy for the design of high efficiency lithium oxygen battery catalysts.

Unlocking the Power of Lewis Basicity in Oxide Lattice Oxygens: A Regulating Force for Enhanced Oxygen Evolution Kinetics in Li-O2 Batteries.

Lithium-oxygen batteries (LOBs) require fast oxygen conversion kinetics to achieve good cycling performance and high energy efficiency. In the text of catalysts for LOBs, Lewis basicity of lattice oxygens (OL) in common transition metal oxides is often underestimated due to the weak electron donor characteristic of OL. In this work, a new spinel-type high entropy oxide with Lewis basicity (LB-HEO) was synthesized through a Joule-heating method. OL was activated by regulating the tetrahedral site-OL-octahedral site (MTd-OL-MOh) units in the spinel-type HEO, enhancing the Lewis basicity. Used as cathode catalyst for LOBs, LB-HEO could attract Li+ and increase the disorder in discharge product, lithium peroxide (Li2O2), promoting the delithiation process and the interfacial charge transfer at the LB-HEO|Li2O2 interface. The activation energy of interfacial charge transfer was significantly reduced from 63.5 kJ mol-1 to 22.4 kJ mol-1. As a result, low charging overpotential of 0.97 V and long cycling lifespan of 135 cycles at 100 mA g-1 were achieved with capacity limitation of 1000 mAh g-1. The strategy based on the regulation of Li+ behavior through its interaction with Lewis bases provides a promising prospective for the design of non-noble metal catalysts for high-performance LOBs.

Spectroscopic Quantitative Analysis of Singlet Oxygen (1O2) in Lithium–Oxygen Batteries during Discharge

Spectroscopic Quantitative Analysis of Singlet Oxygen (¹O₂) in Lithium–Oxygen Batteries during Discharge

Investigating the effect of the textural properties of Zeolite-Templated Carbon Air Electrode on Lithium-Oxygen Battery Performance

Investigating the effect of the textural properties of Zeolite-Templated Carbon Air Electrode on Lithium-Oxygen Battery Performance

Unveiling Oxygen Reaction Mechanisms on Single-Layer Graphene Surface in DMSO-based Electrolyte for Lithium-Oxygen Batteries by in situ EC-AFM Observations

Unveiling Oxygen Reaction Mechanisms on Single-Layer Graphene Surface in DMSO-based Electrolyte for Lithium-Oxygen Batteries by in situ EC-AFM Observations

Innovative MOF linker engineering in PVDF-HFP gel electrolyte matrix for solid-state lithium-oxygen batteries

Innovative MOF linker engineering in PVDF-HFP gel electrolyte matrix for solid-state lithium-oxygen batteries

Cascade reactors for long-life solid-state sodium–air batteries

Sodium (Na)-air batteries show significant potential as alternatives to lithium-air batteries due to their high theoretical energy density and the abundant availability of sodium reserves. Nevertheless, the formation of complex products, specifically NaO2, Na2O2, Na2CO3·xH2O, during the multi-step reactions inevitably raises reconciled potential incompatibility that causes low efficiency and large overpotential. Here, we introduce a cascade electrocatalysis strategy that involves switchable metal and oxygen redox chemistry through electrochemical potential tuning. Leveraging the lithium ion spatial pinning effect, sodium ions trigger in the Na[Li1/3Ru2/3]O2 electrode system to toggle the geometric state at a low electrochemical potential and oscillate among different catalytic states to achieve sequential conversion of complicated multi-step intermediates. The Na[Li1/3Ru2/3]O2 catalyst effectively compartmentalizes the threshold potential that circumvents deactivating or competing pathways while coupling different catalytic cycles. As a result, the sodium-air battery employing this catalyst exhibits long-term reversibility over 1000 cycles with a decent catalysis efficiency exceeding 99%. Our results demonstrate that the cascade electrocatalysis strategy contributes to the design of integrated sodium-air batteries with long-term cycling stability.

Magnetic Field-Driven Catalysis: Revealing Enhanced Oxygen Reactions in Li-O2 Batteries Using Tailored Magnetic Nanocatalysts.

Lithium-oxygen (Li-O2) batteries offer immense promise for next-generation energy storage technology due to their ultra-high theoretical energy density. However, their adoption faces challenges like large overpotential and slow oxygen reaction kinetics. This study introduces a novel strategy that leverages custom-designed magnetic nanocatalysts and external magnetic fields to boost electrochemical performance. Mn-Co-Fe oxide catalysts with adjustable magnetic properties is developed and demonstrated the correlation between the magnetism of the catalysts and the enhancement of battery performance. In the presence of an external magnetic field, the paramagnetic oxygen molecules experience a Kelvin force, while the Li+ ions are influenced by a Lorentz force. This accelerates their diffusion, significantly enhancing the kinetics of both the oxygen reduction and oxygen evolution reactions. The catalyst with the highest magnetization boosted specific capacity by 52.9% (from 8143 to 12455mAhg⁻¹) and significantly lowered the overpotential. This breakthrough underscores magnetic field-driven catalysis as a crucial advancement in unlocking the full potential of Li-O2 batteries, setting new benchmarks for energy storage technology.

Iridium Cluster Decoration on Amorphous Cobalt Oxide-Coated Carbon Nanotubes for High-Performance Lithium-Oxygen Battery Cathodes.

Lithium-oxygen batteries hold great promise for next-generation energy storage due to their exceptionally high theoretical energy density. However, their practical application is hindered by the sluggish kinetics associated with the oxygen reduction reaction and oxygen evolution reaction, resulting in severe voltage polarization and limited cycling stability. Herein, a simple solvent thermal reaction and a one-step reduction reaction is developed, where amorphous cobalt oxide (CoO) is uniformly coated on multi-walled carbon nanotubes (CNT) and further decorated with highly dispersed iridium (Ir) clusters. The amorphous CoO coatings preferentially nucleate at CNT defect sites, which not only passivates surface defects but also facilitates the homogeneous distribution of Ir clusters. This unique Ir/CoO@CNT architecture provides abundant active sites and promotes efficient electronic and ionic transport, thereby enhancing the electrocatalytic activity and overall battery performance. The synergistic effect between the highly active Ir clusters and the amorphous CoO, which accelerates reaction kinetics and stabilizes the electrode interface. As a result, the Ir/CoO@CNT cathode achieves a high discharge capacity of ≈6700mAhg-1, with a low overpotential of 0.96V and exhibits excellent cycling stability, sustaining over 150 cycles under a limited capacity of 500mAhg-1 at 500mAg-1.

Crafting the Organic-Inorganic Interface with a Bridging Architecture for Solid-State Li-O2 Batteries.

Solid-state lithium-oxygen batteries (SSLOBs) are offering unparalleled safety and exceptional electrochemical performance. Despite their promise, composite solid electrolytes (CSEs) fabricated through mechanical hybridization consistently manifest pronounced ceramic particle aggregation. In this study, a thin and flexible CSE is developed by integrating Li10GeP2S12 (LGPS) with poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) and implementing silane coupling agents to form a bridging framework across the organic-inorganic heterojunction interfaces. The engineered CSE exhibited remarkable room-temperature ionic conductivity reaching 1.05×10-4Scm-1, superior electrochemical stability within an expanded voltage window extending to 4.9V versus Li/Li+. Furthermore, lithium symmetrical cells revealed uniform lithium deposition/dissolution behavior over 3000 h. Integration of the thin-film CSE into SSLOBs yielded devices achieving specific discharge capacities of 12874mAhg-1, coupled with superior long-term operational stability throughout 120 cycles. The enhanced interfacial adhesion forces observed between the heterogeneous phases play a pivotal role in maintaining space charge region stability, subsequently promoting accelerated lithium-ion diffusion kinetics while optimizing charge transfer processes at the electrochemical interfaces. The systematic study presents an innovative synthetic strategy for engineering dimensionally-confined, sulfide-enriched CSEs.

Synergistic Zirconium‐Based Metal‐Organic Framework/Reduced Graphene Oxide Nanocomposite as a High‐Efficiency Cathode Catalyst for Rechargeable Lithium‐Oxygen Batteries

Lithium‐oxygen batteries (LOBs) are widely regarded as next‐generation energy storage technologies, owing to their exceptional theoretical energy density (~3500 Wh kg‐1). However, sluggish oxygen redox kinetics and rapid capacity degradation caused by insulating discharge products remain critical challenges. In this study, a hierarchical nanocomposite comprising zirconium‐based metal–organic frameworks (MOF) grown in situ on a three‐dimensional conductive reduced graphene oxide network is strategically fabricated via a solvothermal method. The optimised structure provides abundant active interfaces and efficient electron transport pathways, mitigating electrode surface inactivation and reaction hysteresis. Electrochemical analyses indicate that the composite cathode exhibits a remarkable specific capacity of 16680 mAh g‐1 at 400 mA g‐1 and maintains 193 cycles under fixed‐capacity cycling (500 mA g‐1, 500 mAh g‐1). First‐principles density functional theory (DFT) simulations demonstrate that the interfacial charge redistribution within the composite achieves an optimized LiO2 intermediate adsorption energy of ‐2.31 eV. This represents a substantial moderation compared to the overbinding strength of pristine zirconium‐based MOF and the weak adsorption exhibited by isolated reduced graphene oxide. The composite exhibits intermediate adsorption strength effectively regulates both nucleation and decomposition energetics of discharge products.

Current-Dependent Morphologies of Insulating Electrodeposits in Li-O2 Batteries Controlled by Coupled Ion-Electron Transfer Kinetics.

Lithium-oxygen batteries (Li-O2) present a compelling prospect for the next generation of batteries owing to their exceptionally high theoretical energy density. However, the performance of Li-O2 batteries remains limited by the formation of insulating oxides covering the gas electrode, leading to low capacity or even unexpected sudden death. Existing mathematical models using Butler-Volmer kinetics exhibit uncertainties and inaccuracies in predicting the voltage responses and the morphological evolution of the insulating oxides. In this study, we incorporate coupled ion-electron transfer theory with a phase-field model to enable consistent predictions of the voltage curves, oxide morphologies, and roles of solvation energy. This study provides a valuable predictive tool for the predictive design of electrolytes and electrodes for batteries forming insulating products.

Post-Lithium Battery Technologies Driving the Future of Eco-Conscious Electric Vehicles

As electric vehicles (EVs) transition from niche adoption to mass-market reality, the underlying lithium-ion battery (LIB) architecture has begun to show limitations in cost, safety, and sustainability. This paper presents a comprehensive exploration of emerging post-lithium battery technologies—namely sodium-ion, potassium-ion, magnesium/calcium-ion, aluminum-ion, lithium-sulfur, lithium-air, and solid-state batteries—each promising to address one or more of LIB's systemic flaws. Drawing from recent breakthroughs in materials science and electrochemistry, we examine the technical maturity, environmental implications, commercial viability, and infrastructure requirements for each chemistry. We conclude by identifying critical challenges and strategic pathways for large-scale deployment of these battery systems in pursuit of resilient, low-carbon electric mobility.

Redox Mediators for Li2CO3 Decomposition

Lithium–air batteries (LABs) possess the highest energy density among all energy storage systems, and have drawn widespread interest in academia and industry. However, many arduous challenges are still to be conquered, one of them is Li2CO3, which is a ubiquitous product in LABs. It is inevitably produced but difficult to decompose; therefore, Li2CO3 is perceived as the “Achilles’ heel of LABs”. Among various approaches to addressing the Li2CO3 issue, developing Li2CO3-decomposing redox mediators (RMs) is one of the most convenient and versatile, because they can be electrochemically oxidized at the gas cathode surface, then they diffuse to the solid-state products and chemically oxidize them, recovering the RMs to a pristine state and avoiding solid-state catalysts’ contact instability with Li2CO3. Furthermore, because of their function mechanism, they can double as catalysts for Li2O2/LiOH decomposition, which are needed in LABs/LOBs anyway regardless of Li2CO3 incorporation due to the sluggish kinetics of oxygen reduction/evolution reactions. This review summarizes the progress in Li2CO3-decomposing RMs, including halides, metal–chelate complexes, and metal-free organic compounds. The insights into and discrepancies in the mechanisms of Li2CO3 decomposition and corresponding catalysis processes are also discussed.

Oxygen Vacancy-Rich Ce-Doped NiO Nanorods as Cathode Catalysts for Oxygen Evolution and Lithium–Oxygen Batteries

Oxygen Vacancy-Rich Ce-Doped NiO Nanorods as Cathode Catalysts for Oxygen Evolution and Lithium–Oxygen Batteries

Interface Engineering of Branched PdCoPx Nanostructures for High-Performance Lithium-Oxygen Batteries.

Developing advanced cathode materials plays a positive role in lowering the charge/discharge overpotentials and improving the cycling performance of lithium-oxygen batteries (LOBs). Here we report a direct synthesis strategy to prepare high-dimensional branched PdCoPx series nanostructures, in which the Pd atoms are well dispersed within cobalt phosphide, leading to rich Pd─Co─P interfaces and evoking a prominent ligand effect between the elements. The Pd1Co2Px exhibits an excellent and stable activity for oxygen reduction reaction (ORR) in alkaline media, with a mass activity of 1.46A mgPd -1, far exceeding that of commercial Pd/C (0.12A mgPd -1) and Pt/C (0.17A mgPt -1). Using Pd1Co2Px as the cathode, the resulting LOB shows an ultralow discharge/charge overpotential of 0.40V and could run stably for over 240 cycles, which is a significant improvement compared with the counterparts using CoPx and Pd/C cathodes. Experimental and density functional theory (DFT) calculation results indicate that the dispersed Pd atoms could significantly enhance the ORR kinetics, and the Pd─Co─P interfaces could direct the two-dimensional growth of Li2O2, thereby facilitating the formation of more easily decomposable film-like Li2O2 products. This feature successfully elevates both the charge and discharge performances, as well as the stability of the LOB.

Interface Engineering of Branched PdCoPx Nanostructures for High‐Performance Lithium–Oxygen Batteries

Abstract Developing advanced cathode materials plays a positive role in lowering the charge/discharge overpotentials and improving the cycling performance of lithium–oxygen batteries (LOBs). Here we report a direct synthesis strategy to prepare high‐dimensional branched PdCoPx series nanostructures, in which the Pd atoms are well dispersed within cobalt phosphide, leading to rich Pd─Co─P interfaces and evoking a prominent ligand effect between the elements. The Pd1Co2Px exhibits an excellent and stable activity for oxygen reduction reaction (ORR) in alkaline media, with a mass activity of 1.46 A mgPd−1, far exceeding that of commercial Pd/C (0.12 A mgPd−1) and Pt/C (0.17 A mgPt−1). Using Pd1Co2Px as the cathode, the resulting LOB shows an ultralow discharge/charge overpotential of 0.40 V and could run stably for over 240 cycles, which is a significant improvement compared with the counterparts using CoPx and Pd/C cathodes. Experimental and density functional theory (DFT) calculation results indicate that the dispersed Pd atoms could significantly enhance the ORR kinetics, and the Pd─Co─P interfaces could direct the two‐dimensional growth of Li2O2, thereby facilitating the formation of more easily decomposable film‐like Li2O2 products. This feature successfully elevates both the charge and discharge performances, as well as the stability of the LOB.