Electrode Materials For Batteries Research Articles

Recent advances in conjugated ladder-type porous polymer networks for rechargeable batteries

Owing to the abundant resources, environmental benignity, structural designability, and reasonable theoretical capacity, organic electrode compounds are considered to be an excellent substitute for traditional inorganic electrode materials, which can be applied in green and sustainable recharge batteries. Consequently, organic electrode materials have received considerable attention over the past decade, and numerous organic and polymeric materials have been prepared as high-efficiency electrode materials for batteries. Among them, conjugated ladder-type porous polymer networks (PPNs) with intralayer π-conjugation, interlayer π-π stacking interactions, and rigid backbones have emerged as attractive platforms for rechargeable batteries. This review summarizes the linkage chemistry, synthesis methods, and typical structure of ladder PPNs, the redox activity of the linkage, and their applications in secondary batteries. Further, approaches to enhance the performance and efficiency of these electrode materials are presented. The potential battery applications of the ladder PPNs structure are also discussed.

Two-Dimensional Siloxene Nanosheets: Understanding the Effect of Heat Treatment on the Surface Chemistry and Resulting Electrochemistry in Lithium-Based Batteries.

Two-dimensional (2D) silicon materials are conceptually appealing as negative electrode materials in lithium-ion batteries due to their layered morphology, which can accommodate (de)lithiation-induced volume changes. Herein, heat treatment of 2D Siloxene materials was used to modify the surface functional groups to determine the impact on the electrochemical behavior. Spectroscopic characterization of the heat-treated nanosheets confirmed the loss of oxygenated and hydride surface functional groups with an increased annealing temperature. Formation and disproportionation of the amorphous suboxides with increasing heat treatment were affirmed with lab and synchrotron-based measurements. A reduced irreversible capacity was observed for Siloxene with a higher temperature heat treatment consistent with the formation of a more favorable surface electrolyte interphase (SEI). A Siloxene-400||NMC622 full cell (prepared with 400 °C-annealed Siloxene (Siloxene-400) and LiNi0.6Mn0.2Co0.2O2 (NMC622)) showed significantly enhanced capacity and rate capability compared to a nano Si||NMC622 cell. These results illustrate the ability of thermal annealing to modify the surface functional groups of Siloxene and highlight the favorable impact of the appropriate surface functionality on the electrochemistry of Siloxene in lithium cells.

Multi-anionic and multi-cationic high-entropy oxides as electrode materials for lithium-ion batteries

Multi-anionic and multi-cationic high-entropy oxides as electrode materials for lithium-ion batteries

Recent experimental and theoretical progress in silicene based electrode materials for rechargeable batteries and supercapacitors

Recent experimental and theoretical progress in silicene based electrode materials for rechargeable batteries and supercapacitors

Structural water and composing with graphene synergistically boosting electrochemical lithium-storage performance of hydrated tungsten oxides

Structural water and composing with graphene synergistically boosting electrochemical lithium-storage performance of hydrated tungsten oxides

Study for the construction of CoMoO4 rod-like microstructures as anode material for high rate lithium-ion batteries

Study for the construction of CoMoO4 rod-like microstructures as anode material for high rate lithium-ion batteries

DFT and AIMD studies of SnFe2O4 as a promising anode for Li-ion batteries

DFT and AIMD studies of SnFe2O4 as a promising anode for Li-ion batteries

In-situ grown CoVSe/reduced graphene oxide nanocomposites as bifunctional electrode material for supercapacitors and lithium-ion batteries

In-situ grown CoVSe/reduced graphene oxide nanocomposites as bifunctional electrode material for supercapacitors and lithium-ion batteries

A Novel KTP-Type NaTiPO4F electrode material for High-Performance Na-Ion Batteries

A Novel KTP-Type NaTiPO4F electrode material for High-Performance Na-Ion Batteries

Design and synthesis of nickel-cobalt-aluminum hydroxide battery electrode materials for high-performance hybrid supercapacitors

Design and synthesis of nickel-cobalt-aluminum hydroxide battery electrode materials for high-performance hybrid supercapacitors

Unleashing high‐efficiency proton storage: Innovative design of ladder‐type organic molecules

AbstractThe architectural design of redox‐active organic molecules and the modulation of their electronic properties significantly influence their application in energy storage systems within aqueous environments. However, these organic molecules often exhibit sluggish reaction kinetics and unsatisfactory utilization of active sites, presenting significant challenges for their practical deployment as electrode materials in aqueous batteries. In this study, we have synthesized a novel organic compound (PTPZ), comprised of a centrally symmetric and fully ladder‐type structure, tailored for aqueous proton storage. This unique configuration imparts the PTPZ molecule with high electron delocalization and enhanced structural stability. As an electrode material, PTPZ demonstrates a substantial proton‐storage capacity of 311.9 mAh g−1, with an active group utilization efficiency of up to 89% facilitated by an 8‐electron transfer process, while maintaining a capacity retention of 92.89% after 8000 charging‐discharging cycles. Furthermore, in‐situ monitoring technologies and various theoretical analyses have pinpointed the associated electrochemical processes of the PTPZ electrode, revealing exceptional redox activity, rapid proton diffusion, and efficient charge transfer. These attributes confer a significant competitive advantage to PTPZ as an anode material for high‐performance proton storage devices. Consequently, this work contributes to the rational design of organic electrode materials for the advancement of rechargeable aqueous batteries.

First-Principles Approach to Assess the Viability of MoOPO4 as an Electrode Material for Mg-Ion Batteries

First-Principles Approach to Assess the Viability of MoOPO₄ as an Electrode Material for Mg-Ion Batteries

Multi-Dimensional Inorganic Electrode Materials for High-Performance Lithium-Ion Batteries

Energy storage devices are essential for enhancing the effectiveness and sustainability of electrical energy. Lithium-ion batteries (LIBs) are one of the most efficient energy storage solutions available. The choice of electrode materials plays a vital role in defining the performance of an energy storage device. A range of electrode materials have been developed utilizing both organic and inorganic substances. Due to their notable electrochemical characteristics, strong chemical stability, and well-established technological approaches, inorganic materials have been extensively studied to achieve high-performance devices. This review paper aims to provide a thorough and analytical review of different materials ranging from zero- to three-dimensional (3D), like quantum dots, nanotubes, and nanosheets that have been proposed for high-performance LIBs. This study also includes challenges and future pathways to address the issues with inorganic materials utilized as electrode materials for high-performance energy storage LIBs.

Thermal processing to modulate surface chemistry and bulk charge distribution in nickel-rich layered lithium positive electrodes

The broader application of nickel-rich layered oxides as positive electrode materials for lithium-ion batteries has been hindered by their high manufacturing cost and inferior cycling stability. Thermal processing, which is integral to electrode materials manufacturing and fundamental in materials science, has not been fully utilized to design advanced positive electrode materials. Herein, we demonstrate the capability of using quenching heat treatment to regulate Li distribution and modulate electronic structure near particle surface. The resulting materials exhibit less parasitic reactions with the electrolyte and an improved charge distribution homogeneity in secondary particles, leading to more stable cycling performance at high voltages (4.5 V vs Li/Li+). Our synchrotron X-ray analyses reveal the underlying interplay between surface structure and bulk charge distribution in positive electrode materials particles. While strategies used to stabilize positive electrode materials through compositional control, surface modification, and electrolyte engineering have become mature, thermal processing can be advantageous to further improve positive electrode materials manufacturing.

Li-ion storage characteristics and migration mechanisms of intrinsic, doped, and oxygen-deficient CeO2 and La2O3: A study using DFT+U

Rare-earth oxides (REOs) represented by CeO2 and La2O3 became a focal point in the study of Li-ion battery (LIB) electrode materials. However, leveraging defects to tune the intrinsic electronic structure of REO to enhance electrochemical performance, as well as understanding the underlying physical mechanisms at the atomic level, remained an open challenge. Density functional theory plus U calculations revealed that doping and oxygen vacancies not only regulated Li-ion insertion stability but also reduced the migration energy barriers in CeO2. Doping also decreased the volume change rate of CeO2 during Li-ion insertion. Oxygen vacancies lowered the Li-ion migration energy barrier in CeO2 from 1.516 to 0.903 eV. In comparison, Li-ion migration energy barriers in the La2O3 series structures were significantly lower than those in CeO2. Experimental results confirmed that the Li-ion diffusion coefficient of La2O3 was markedly higher than that of CeO2. Upon Li-ion insertion, the bandgap of CeO2 decreased from 2.18 to 1.60 eV, and density of states analysis revealed the profound impact of lithiation on the electronic structure. This comprehensive study enhances the understanding of the application potential of these typical rare-earth oxide materials in LIBs.

Poly(1,4‐anthraquinone) as an Organic Electrode Material: Interplay of the Electronic and Structural Properties due to the Unusual Lone‐Pair‐π Conjugation

AbstractOrganic semiconductors with lone‐pair‐π conjugation offer a promising yet enigmatic route to advanced electrode materials for rechargeable batteries. This study employs molecular dynamics and electronic structure simulations to explore the relationship between structural and electronic properties of poly(1,4‐anthraquinone) (P14AQ), which exhibits this unusual conjugation mechanism. The results indicate that P14AQ is resistant to structural disorder, always maintaining an appreciable conjugation within its polymer chain. It also shows restrained volume changes when lithium, magnesium, and hydrogen cations are intercalated during battery cycling. These results rationalize the reported good performance of P14AQ as an organic cathode material. The analysis offers fundamental insights into the role of lone‐pair‐π conjugation in organic semiconductors and paves the way for developing new materials based on this unorthodox design paradigm.

Image registration for accurate electrode deformation analysis in operando microscopy of battery materials

Operando imaging techniques have become increasingly valuable in both battery research and manufacturing. However, the reliability of these methods can be compromised by instabilities in the imaging setup and operando cells, particularly when utilizing high-resolution imaging systems. The acquired imaging data often include features arising from both undesirable system vibrations and drift, as well as the scientifically relevant deformations occurring in the battery sample during cell operation. For meaningful analysis, it is crucial to distinguish and separately evaluate these two factors. To address these challenges, we employ a suite of advanced image-processing techniques. These include fast Fourier transform analysis in the frequency domain, power spectrum-based assessments for image quality, as well as rigid and non-rigid image-registration methods. These techniques allow us to identify and exclude blurred images, correct for displacements caused by motor vibrations and sample holder drift and, thus, prevent unwanted image artifacts from affecting subsequent analyses and interpretations. Additionally, we apply optical flow analysis to track the dynamic deformation of battery electrode materials during electrochemical cycling. This enables us to observe and quantify the evolving mechanical responses of the electrodes, offering deeper insights into battery degradation. Together, these methods ensure more accurate image analysis and enhance our understanding of the chemomechanical interplay in battery performance and longevity.

Extreme Defect Tolerance for Electrochemical Intercalation in Wadsley-Roth Structures Demonstrated by Metastable NaNb7O18.

Careful control over the defect chemistry of crystalline compounds is typically critical to transport phenomena (ion, electron, phonon). In one-dimensional (1D) ion conductors, even small concentrations of defects in the diffusion pathway can be pernicious. Wadsley-Roth block phases are 1D ion conductors with high redox capacity and among the highest diffusivity of any battery electrode materials. The origin of their high-rate transport has been attributed to parallel tunnels that could impart defect tolerance, but direct evidence is limited. Herein, a new lithium-ion battery negative electrode material, NaNb7O18, is described that exhibits extreme defect tolerance. Multimodal characterization combining neutron diffraction, 23Na solid-state NMR spectroscopy, and DFT calculations reveals that more than half of the Na+ in NaNb7O18 is in diffusion tunnel-blocking cuboctahedral environments (similar to the perovskite A-site). Despite the high point-defect concentration, NaNb7O18 can reversibly lithiate to Li7NaNb7O18 and cycle 200 mAh·g-1 in 10 h and 100 mAh·g-1 in 3 min in large 4-23 μm (D10-D90) particles. Operando synchrotron diffraction shows an anisotropic and asymmetric lithiation/delithiation process with two first-order phase transitions including one with nearly zero volume change. LixNaNb7O18 also exhibits evidence for reversible Nb-Nb bond formation. From the same operando diffraction measurements, Nb-Nb distances between edge-sharing octahedra at the block peripheries vary from ca. 3.4 to 2.8 and back to 3.4 Å over one lithium insertion/extraction cycle, in quantitative agreement with the Nb-Nb bond formation charge storage mechanism recently proposed from the computational lithiation of several different Wadsley-Roth compounds.

High performance of air plasma-exposed MgCo2O4 electrode material for rechargeable Mg batteries and supercapacitors

High performance of air plasma-exposed MgCo2O4 electrode material for rechargeable Mg batteries and supercapacitors

Improving Sodium Manganese Hexacyanoferrate with Optimized Synthesis Conditions, Effective Drying, and Small Amounts of Nickel

Prussian Blue Analogs are a promising class of positive electrode materials for sodium-ion batteries that can be synthesized at low temperatures using only Earth-abundant elements like sodium, iron, and manganese. Their open framework structure allows them to sustain high current densities but also makes them prone to absorption of moisture. We improve the specific capacity of sodium manganese hexacyanoferrate (MnHCF) by optimizing synthesis and processing conditions, enabling a material-level energy density of 562 Wh kg−1, which is on par with lithium iron phosphate. We remove interstitial water from these materials by rigorous drying. We also demonstrate a factor two improvement in cycling life of MnHCF by substituting only 3 at. % Ni for Mn and leaving some vacancies, which leads to 80% capacity retention after 3,500 h (∼5 months) of cycling in Na half cells at 0.2 C between 2.0 and 4.1 V and an ability to retain >85% capacity at a high current density of 10 C.