The performance of solid-state lithium-ion conductors is fundamentally governed by their conduction mechanisms. This talk introduces a materials-by-design strategy to optimize both ionic conductivity and lithium-ion transference number through deliberate control of ion transport pathways. Polyethylene oxide (PEO)-based conductors typically rely on segmental motion, resulting in low ionic conductivity and low lithium transference numbers. Ion hopping mechanisms can achieve high lithium transference numbers but suffer from limited conductivity due to long hopping distances and elevated energy barriers. In contrast, the vehicle mechanism offers a promising route to simultaneously attain high ionic conductivity and high lithium transference number, presenting a compelling direction for advancing solid-state electrolytes. These results have important implication in design of polymer and composite electrolytes for lithium-ion batteries.
Interface integration is crucial for achieving rapid lithium-ion transport and conversion under high mass loading and represents a key strategy for constructing high-energy-density quasi-solid-state lithium metal batteries (QSSLMBs). However, Li deposition at the electrode interface during cycling tends to generate significant mechanical stress, leading to interface delamination, increased impedance, and rapid battery failure. Herein, we design a mixed ionic-electronic conductive composite anode by integrating gel electrolyte into a three-dimensional hollow MXene/Li scaffold. This architecture enables dynamic volume accommodation while guiding uniform Li deposition into internal cavities via lithiophilic sites and curved pore geometry, effectively suppressing dendrite growth and interfacial stress. The resulting all-in-one QSSLMBs achieve over 1750 h in symmetric cells and maintain 72.6% capacity after 1000 cycles at 1 C in a LiFePO4 full cell. When paired with a high loading LiNi0.9Co0.05Mn0.05O2 cathode (31.5 mg cm-2), a single-layer and projected 13-layer pouch cells achieve an energy density of 392 Wh kg-1 and 561 Wh kg-1, demonstrating its potential for durable, high-energy QSSLMBs.
The practical application of lithium (Li) metal anodes is severely hindered by uncontrolled dendrite growth and infinite volume changes, particularly under high‐rate cycling conditions. Herein, we propose a robust mechanically interlocked Li‐phosphor bronze mesh (Li@PBM) composite anode for high‐rate Li metal batteries (LMBs), fabricated via a facile mechanical rolling process. Both experimental characterizations and phase‐field simulations reveal that the active Sn and P species within the PBM trigger an in situ interfacial reconstruction, which significantly enhances the chemical affinity toward Li. Synergistically, the unique mechanical interlocked structure accommodates volume fluctuations and redistributes the local electric field, guiding uniform Li deposition even at high current densities. Consequently, the Li@PBM||Li@PBM cells demonstrate exceptional cycling stability for over 1000 h at 5 mA cm−2 and 5 mAh cm−2, whereas the Li||Li cells suffer from large voltage hysteresis and fail within 100 h. Furthermore, pairing with LiFePO4 (LFP) cathodes (11.2 mg cm−2), the LFP||Li@PBM cells achieve 83.5% capacity retention over 500 cycles at 5.0 C (0.75 A g−1). In contrast, the LFP||Li counterparts experience rapid capacity decay, retaining only 53.1% capacity after 200 cycles. This work highlights the efficacy of combining alloy chemistry with structural engineering to unlock the potential of high‐rate LMBs.
The integration of high-penetration residential photovoltaics (PVs) into low-voltage distribution networks (LVDNs) presents significant challenges to conventional voltage regulation devices, such as on-load tap changer (OLTC) and capacitor banks (CBs), in mitigating voltage violations at terminal buses. Given the great regulation potential of demand-side flexible resources, including battery energy storages (BESs), thermal energy storages (TESs), and thermostatically-controlled loads (TCLs), this paper proposes a two-stage optimization strategy to coordinate diverse VRRs in LVDNs. In the first stage, the second-order cone programming (SOCP) is employed to obtain optimal operation schedule of OLTC and CBs. In the second stage, a distributed algorithm is designed for the multi-energy storage (MES) cluster consist of BESs, TESs, and TCLs to participate in auxiliary voltage regulation, where Adam algorithm is utilized to accelerate convergence speed and enhance robustness. Finally, a modified Danish 11-bus system is built to validate the control performance of proposed method. The results demonstrate its effectiveness in voltage regulation under scenarios with PV generation and load demand uncertainties.
ABSTRACT Layered oxide cathodes are a leading class of high‐energy‐density electrode materials for lithium‐ion batteries, but their long‐term stability at high voltages is compromised by chemical corrosion and mechanical stress at grain boundaries. Here, we report the construction of an elastic and voltage‐tolerant poly(urea‐siloxane) (PUSi) coating via the in situ polymerization of amine‐terminated polydimethylsiloxane and toluene diisocyanate (TDI). This polymer acted as a conformal artificial interphase that stabilized the secondary‐particle surface and internal primary‐particle surfaces. The PUSi layer acted as a stable chemical barrier that isolated cathode interfaces from direct contact with the electrolyte. This suppressed interfacial side reactions and inhibited the layered‐to‐spinel phase transformation. The tailorable elasticity of the PUSi layer allowed it to accommodate cyclic volumetric variations and suppress intergranular cracking during high‐voltage cycling. When applied to LiNi 0.6 Co 0.2 Mn 0.2 O 2 , the cathode showed a capacity retention of 81.2% after 450 cycles in coin cells and 82.4% after 200 cycles in Li‐metal pouch cells under a cut‐off voltage of 4.5 V. The generality of this approach was demonstrated by using it to coat LiNi 0.8 Co 0.1 Mn 0.1 O 2 and lithium‐rich layered oxides. This work provides a scalable and eco‐friendly route for engineering grain boundaries and interfacial stability in high‐energy cathode systems.
The increasing integration of power electronic converters in modern power systems has significantly accentuated stability concerns. Among these, the synchronization stability challenges of grid-following (GFL) converters under weak grid conditions are particularly prominent. It has been demonstrated that the introduction of grid-forming (GFM) converters can effectively mitigate these stability issues. However, a theoretical understanding of how various GFM control strategies impact GFL stability is still incomplete, making the small-signal stability assessment of hybrid GFL-GFM systems a significant challenge. Moreover, the reactive power control (RPC) of GFM converters plays a crucial role in maintaining system stability. Research on how RPC affects its support capability remains unexplored. To address these issues, this paper proposes a stability assessment method for GFL-GFM hybrid systems. By employing modal decoupling and matrix perturbation methods, a decoupled low-order system is developed for characterizing the stability of the original system, thereby reducing the analytical complexity and offering physical insights into the supporting capabilities of GFM converters. Furthermore, an enhanced RPC structure for GFM converters is proposed to improve their grid-support capability within different frequency ranges. The effectiveness of the proposed method is validated on the IEEE 39-Node system.
Photoelectrochemical (PEC) sensors integrate light excitation with electrochemical detection, providing low background noise and robust anti-interference capabilities. Surface plasmon resonance (SPR) acts as an effective light antenna for signal transduction in these sensors. Traditionally, plasmon-mediated PEC sensors operate via hot carrier injection, which necessitates direct contact between the plasmonic antenna and the semiconductor, thereby limiting sensor design flexibility. In this work, we introduce plasmon-induced resonance energy transfer (PIRET) as a novel signal transduction mechanism in a PEC immunosensor. A Bi _3 FeMo _2 O _12 (BFMO) semiconductor thin film is functionalized with capture antibodies, while plasmonic Au nanoparticles with absorption spectrum overlapping with BFMO are conjugated to detection antibodies. Upon target antigen binding, the Au nanoparticles are positioned in proximity to the BFMO surface through a sandwich immunoassay configuration, enabling PIRET-mediated generation of electron-hole pairs in BFMO. Using human IgG as a model analyte, we demonstrate the feasibility and advantages of PIRET, highlighting its potential to extend PEC sensor design by permitting a physical gap between the plasmonic antenna and semiconductor.
The formation of zinc dendrites is a significant obstacle to commercializing zinc-ion batteries. Although the discrepancy between the fast electrochemical reaction kinetics and the comparatively sluggish mass transfer leads to the formation and growth of dendrites, a profound understanding of how the relationship between the two factors influences dendrite formation is essential. Here, through investigating a series of urea derivatives for regulating Zn2+ plating, we find that achieving a better balance between electrochemical reaction kinetics and the mass transfer rate is crucial for effectively suppressing dendrite formation. A dimensionless constant, K, is proposed to quantify the balance between these two factors. As a result, the electrolyte with N, N-dimethylurea has the highest K value, enabling cumulative capacities of 11,000 mAh cm-2 for Zn | |Zn cells and 7,500 mAh cm-2 for Zn | |Cu cells achieved at a current density of 10 mA cm-2. Furthermore, the Zn | |Zn0.25V2O5·nH2O pouch cell with a mass loading of 60 mg cm-2 delivers a capacity of 6.95 Ah and demonstrates stable cycling performance using the modified electrolyte. This work provides theoretical insights into governing the formation and growth of zinc dendrites.
Fast-charging and durable sodium-ion batteries (SIBs) with high volumetric energy density (VED) hold particular promise for large-scale electrification, but are fundamentally hindered by slow Na + diffusion dynamics, structural and interfacial instabilities of conventional anodes. Here we simultaneously address these challenges by pioneering a high-performing bismuth@carbon composite anode featuring a two-dimensional layered micro/nano-hierarchical structure (Bi@C-MMS). Unlike conventional spherical or bulk architectures with uncontrolled deformation and tortuous ion paths, this designed lamellar architecture regulates inherently uncontrolled Bi volume expansion into a well-guided, thickness-directionally confined “breathing” mode while enabling rapid, directional percolating pathways for ion/electron transport. Accordingly, the Bi@C-MMS achieves stress relaxation, durable electrical connectivity, and robust structural/interphase integrity throughout cycling. Pairing with a commercial ultrathick Na 3 V 2 (PO 4 ) 3 cathode (25.81 mg cm − 2 ), the full cells achieve an ultrahigh VED of 391.4 Wh L⁻ 1 . Remarkably, the pouch cell sustains ultrahigh-rate operation at 30 C and stable cycling for over 5000 cycles under 10 C fast-charging conditions. This work provides a guiding principle in practical high-rate, durable and dense alloy anode design for next-generation fast-charging, high-energy batteries.
With the increasing penetration of renewable energy sources and power electronic converters, the grid strength and inertia of modern power systems have significantly declined, potentially leading to various stability challenges, such as small-signal stability and frequency stability. It is widely recognized that the integration of grid-forming (GFM) energy storage systems (ESS) can mitigate these issues and enhance the stable operation of power systems from multiple perspectives. However, determining the optimal configuration of GFM ESS in hybrid systems to balance stability and economic efficiency remains an open research question. To bridge this gap, this paper proposes an optimization method for GFM ESS configuration considering stability constraints. First, based on the small-signal model of the multi-converter system, the relationship between system stability and the placement and capacity of GFM ESS is established, and stability criteria are derived. On this basis, both small-signal stability constraints and inertia constraints are incorporated, formulating the GFM ESS configuration problem as a mixed-integer programming problem. Finally, a relaxation method for eigenvalue constraints and a two-layer iterative algorithm are proposed to solve the optimization problem efficiently. Case studies conducted on the IEEE 39-bus system and the fully inverter-based system validate the accuracy and general applicability of the proposed configuration method.
O3-type layered oxide cathodes suffer from surface chemical instability and sluggish Na+ transport within the O-type framework, limitations that are aggravated by humid-air exposure and fast-charging operation, leading to severe interfacial degradation and rapid capacity decay. Herein, we propose a mild ethylene-glycol-assisted treatment that in situ constructs a coherent surface-to-bulk architecture within NaNi1/3Fe1/3Mn1/3O2 (NFM) particles, comprising a nanoscale surface rock-salt layer, a depth-dependent Na-vacancy gradient, and a Na-deficient bulk. This hierarchical configuration locks the surface chemistry while opening continuous Na+ percolation pathways across the surface-bulk junction, thereby flattening radial (de)sodiation heterogeneity and steering a more uniform, highly reversible phase evolution during prolonged cycling. As a result, the modified sample exhibits outstanding fast-charging performance, delivering 107.6 mAh g-1 at 5C (600 mA g-1) with 81.6% capacity retention after 400 cycles. This work highlights gradient interphase coupled with Na-vacancy engineering as an effective strategy to develop high-performance layered oxide cathodes for sodium-ion batteries.
Optically transparent electromagnetic interference (OTEMI) shielding materials are garnering significant attention due to their dual capabilities of providing electromagnetic interference (EMI) shielding while maintaining optical transparency. Beyond high shielding efficiency, the materials also require lightweight, ultra- thinness, flexibility, and reliability for extreme conditions applications like industrial and aerospace scenarios, which challenges most existing EMI shielding materials. Herein, we utilize the openings in the percolating silver nanowires network to realize the interpenetrating crosslink of polyamide acid, which enables the in-situ, damage-free encapsulation of the vulnerable conductive network and forms a lightweight OTEMI shielding film with exceptional stability. The 8 mu m EMI shielding films show 29-46 dB shielding effectiveness in the 12-18 GHz range, with variable visible light transmittance (45 %-86 %@550 nm), while being capable of withstanding a broad temperature variation from 220 degrees C to- 170 degrees C. Moreover, the solution-processed film possesses excellent bending stability and chemical corrosion resistance, showing its unique applications in harsh conditions inaccessible to humans.
Semiconductor heterojunctions composed of stacked two-dimensional (2D) materials hold great promise for electronics and optoelectronic devices. Hexagonal boron nitride (h-BN) serves as the encapsulation layer that enhances the optical properties of heterojunctions by suppressing interfacial charge scattering and enabling quantum-confined energy transfer. Nevertheless, a mechanistic understanding of the modulation effect of interlayer coupling and interfacial charge dynamics in these heterostructures remains insufficient. Here, we report the in situ growth of ultrathin MoS2 flakes encapsulated within porous h-BN fibers and construct high-quality h-BN/MoS2 heterojunctions, demonstrating defect-mediated interactions and tunable optoelectronic properties. The cross-sectional architecture with the encapsulating sites in porous h-BN confirmed intimate interlayer contact, and investigations via femtosecond transient reflectance spectroscopy revealed the exciton radiative lifetime and defect-mediated charge transfer in the heterojunctions. The photoexcited carriers transfer between long-lived defect states in h-BN and the MoS2, which induces the defect-related PL quenching in h-BN and prolonged radiative lifetime of MoS2 excitons by 3-fold. This was attributed to defect-mediated charge transfer in MoS2 and the dielectric screening from h-BN. This work elucidates the critical role of defect-engineered interfacial charge transfer in h-BN/MoS2 heterostructures, offering valuable insights for advancing optoelectronic devices based on 2D heterojunctions.
Realizing durable, uniform, and dendrite‐free sodium metal deposition is crucial for preventing premature battery failure caused by internal short circuits, which is primarily governed by ion transport and desolvation kinetics during the electrodeposition process. Herein, a composite quasi‐solid polymer electrolyte (LPQSE) is developed through in situ polymerization of poly(ethylene glycol) diacrylate within a porous membrane constructed by in‐house synthesized α‐LiAlO 2 @γ‐Al 2 O 3 (LAO) nanosheets and poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVHF). The LAO nanosheets effectively immobilize PF 6 − anions via Lewis acidic sites, while the PEGDA carbonyl groups coordinate Na⁺ cations. This dual‐interaction mechanism simultaneously reduces ion‐pair formation and promotes loose solvation structures, thereby accelerating desolvation kinetics and significantly increasing sodium nucleation density. Consequently, homogeneous sodium deposition with fundamentally suppressed dendrite nucleation is realized. As a result, solid‐state Na||Na symmetric cells demonstrate exceptional cycling stability, and Na 3 V 2 (PO 4 ) 3 (NVP)||Na batteries employing the ∼16‐µm‐thick LPQSE exhibit long‐term cycling stability. Notably, the NVP||Na battery exhibits a high specific discharge capacity of 69.5 mAh g −1 at 10 C and retains 88.7% capacity retention over 1000 cycles at 1C. This work establishes an innovative electrolyte design strategy that strategically coordinates anion immobilization and cation solvation to regulate deposition behavior for achieving dendrite‐free sodium anodes.
Ni-rich layered oxide (NRLO) materials are considered highly promising cathode for lithium-ion batteries. However, their practical application is limited by capacity loss and interface instability caused by chemical and mechanical failure during cycling. Doping has been identified as a direct and effective method to address these challenges. However, mechanistic understanding of doping enhanced electrochemical performance is still unclear. In this study, the introduction of high-valent Nb ions was employed to achieve mechanical–chemical coupling regulation, thereby concurrently improving the capacity and cycle life of NRLO. First, Nb 5+ doping was conducted to refine secondary grains, achieving a “grain refinement” effect similar to that in ceramics and alloys, while further stabilizing the grain boundaries. The intergrain fusion structure of NCM811-0.5Nb effectively dissipates lattice strain under highly delithiated state, suppresses oxygen loss, and prevents cracks that lead to fracture during cycling. Moreover, Nb doping stabilizes the monoclinic phase during phase transitions and promotes the formation of highly stable spinel twin boundaries after cycling. This effectively reduces the Li diffusion barrier, leading to improved reversible specific capacity and rate capability. Lastly, the strong Nb─O bonding restrains oxygen release and transition metal/Li antisite mixing, thus mitigate rock-salt phase formation. This study demonstrates a comprehensive understanding of the concurrent capacity and stability enhancement mechanisms attributed to Nb-doping and highlights the significant potential of the synergistic regulation of mechanical and chemical coupling in improving the capacity and lifespan of NRLOs by Nb-doping.
Lithium metal batteries (LMBs) are considered promising candidates for high-energy-density energy storage. However, the practical application of lithium (Li) metal anodes is highly constrained by the limited ionic conductivity, localized electronic leakage, and poor mechanical stability of their solid electrolyte interphase (SEI). Herein, a Li-Sr-N (LSN) anode is fabricated by mechanically rolling Sr3N2 powder with Li foil, forming a LiSrN/Li3N/Li23Sr6/Li heterointerface on the foil surface. As demonstrated by both experimental characterizations and theoretical calculations, the as-constructed heterointerface can actively interact with the fluoroethylene carbonate (FEC) molecules in the electrolyte, leading to the in situ formation of a uniform Li3N/LiF/SrF2-hybrid SEI with high ionic conductivity and electronic insulation. With this design, the LSN||LSN symmetric cell exhibits stable cycling performance over 1000 cycles at 1 mA cm-2 and 1 mAh cm-2 in carbonate-based electrolytes. The NCM95||LSN coin-type full cell with an ultrahigh loading cathode (approximate to 18 mg cm-2) achieves 89.6% capacity retention over 100 cycles at 1.0 C (214 mA g-1). Furthermore, the NCM95||LSN pouch cell with a low N/P ratio (approximate to 1.7) and lean electrolyte (approximate to 1.37 g Ah-1) delivers a high energy density of approximate to 440.8 Wh kg-1 and maintains 91.1% capacity retention after 100 cycles at 0.2 C.
The stress distribution in Li metal strongly affects the interfacial Li-ion diffusion, thereby influencing the morphology of plated Li and the performance of the battery. Here, we report a mechano-electrochemical coupling strategy that utilizes an arched structured carbon aerogel to achieve stable Li-plating/stripping electrochemistry. The arch-structured carbon aerogel can actively regulate stress distributions in response to the compressive stresses induced by Li deposition, generating the transition of stress from compressive on the convex surface to tensile on the concave surface, which can effectively promote the Li-migration kinetics and thus suppress the non-uniform deposition of Li. The carbon aerogel with synergistically enriched-oxygen vacancies on its surface boosts rapid interfacial Li-ion migration by reducing the Li+ migration barrier. The non-dendritic Li-metal anode demonstrates smaller electrode level volume variation (<3%), higher coulombic efficiency (98.5%) and a longer cycle lifetime (2000 h at 1 mA cm-2) than conventional planar substrates. A full cell based on the LiFePO4 cathode shows a high capacity retention of 90.2% after 300 cycles at 1 C. The carbon-aerogel/Li|sulfurized polyacrylonitrile full cell delivers a reversible capacity of 1130 mA h g-1 over 270 cycles at 0.2 C. This work reveals a stress-driven dendrite growth suppression mechanism and provides insights into the design of dendrite-free metal anodes for rechargeable metal batteries.
To design high-performance solid-state organic Li-ion conductors, it is essential to shift the paradigm of design from segmental motion mechanisms to new ion transport mechanisms. In this work, we designed a solid-state polymer composite Li-ion conductor that enables the transport of lithium ion but immobilizes anion in lithium salts. This new solid polymeric composite has achieved high ionic conductivity at room temperature and high Li-ion transference number simultaneously. A full-cell battery has been constructed with the use of this new solid polymer electrolyte, which showed high energy density and good cyclic stability. This work has an implication in the design of solid polymer electrolytes for solid-state lithium-ion batteries.
High-nickel LiNi0.83Co0.12Mn0.05O2 (NCM83) cathodes suffer from interfacial instability resulting from cathode-electrolyte reactions and anisotropic mechanical strain within secondary particles. Herein, we present a mechanically adaptive cathode-electrolyte interphase (CEI) engineered via a dynamic covalent network that features a supramolecular ion-conducting polyurethane ureido-pyrimidinone (SPU-UPy) elastomer. The dynamic network integrates cooperative hydrogen bonds and disulfide bonds and imparts exceptional mechanical resilience and autonomous self-healing capabilities that allow it to accommodate volume fluctuations without compromising structural integrity. The SPU-UPy layer is also designed with strong transition metal ion-O/N coordination bonds that greatly enhance adhesion to the NCM83 surface and mitigate transition metal dissolution in the electrolyte. The polyether backbone facilitates efficient Li-ion transport across the interface and ensures a homogeneous interfacial Li concentration during intercalation/deintercalation. Consequently, the dynamic CEI-coated NCM83 cathodes achieve exceptional long-term cycling stability with a high-capacity retention of 82.2% after 400 cycles at 1 C. This work elucidates the critical role of dynamic covalent chemistry in stabilizing Ni-rich cathode interfaces and establishes a new paradigm for the design of high-energy-density batteries through mechano-adaptive interfacial engineering.