Latest ArticlesCharge transfer cocrystals offer an opportunity to construct high performance organic photothermal materials and hold great promise toward various applications, including photothermal imaging, photothermal therapy, seawater desalination. However, the photothermal cocrystal materials are still in infancy and it is necessary to further explore them and develop more novel applications. Herein, a charge transfer cocrystal of anthracene and 7,7′,8,8′-tetracyanoquinodimethane was constructed and has a strong D−A interactions and a small HOMO−LUMO gap (1.46 eV) and thus displays a broad absorption over 300–821 nm range. The near-infrared photothermal conversion performance was evaluated under 808 nm laser illumination and the conversion efficiency reaches 58.3%, with the temperature increases to 72.1 ℃ in 145 s. The cocrystal was successfully employed as a versatile photothermal material for imaging and functional electrical device control, paving the way for the development of emerging applications in related fields.
The oxygen evolution reaction (OER), as the rate-determining step in water electrolysis, demands efficient non-precious catalysts to replace conventional Ru/Ir-based materials. While transition metal sulfides (TMS) show promise application prospect, but is limited by sulfur leaching-induced degradation. We address this challenge through a cyanide-mediated stabilization strategy, developing a Ni-CN/Ni3S2 catalyst where sacrificial C≡N groups transform into C═O moieties during OER. This structural evolution effectively suppresses sulfur leaching while enabling the formation of highly active Ni-SO4-OH species rather than conventional NiOOH. The optimized catalyst demonstrates exceptional performance with a 209 mV overpotential at 10 mA/cm2, outperforming both RuO2 (241 mV) and pristine Ni3S2 (311 mV), and maintains 200 h stability at 100 mA/cm2. When integrated into an anion exchange membrane (AEM) electrolyzer, the catalyst achieves 1 A/cm2 at 1.71 V with 200 h durability (35 µV/h voltage decay). Combined experimental and theoretical analyses reveal that the sulfur-anchored structure enables exceptional stability through controlled surface reconstruction and suppressed element dissolution. This work provides critical insights into designing durable, high-performance OER electrocatalysts through dynamic interface engineering.
Metal-oxo clusters (MOCs), particularly those with renowned Keggin-type architecture, have been extensively studied for their facile synthesis, robust stability, and diverse applications. However, the isolation of thorium-oxo clusters with novel structural motifs remains elusive due to the distinctive hydrolytic behaviour of Th4+ ions. Herein, we report nine electropositive α-Keggin-type thorium-oxo clusters, M@Th12@L8 (where M is fully or co-occupied by Al3+, W6+, Mo6+, V5+, Cr3+, or Mn4+; L = Al or Ga), synthesized via aluminate-regulated Th4+ hydrolysis. Unlike Th6(O/OH)8-based structures for most reported thorium-oxo clusters, M@Th12@L8 features an unprecedented triple-layered Platonic architecture: a central MO6 octahedron, a Th12 icosahedron, and an outer cube of eight LO5 ligands. Structural rigidity maintains invariant M–O bond lengths despite variable MO6 and LO5 units, while the central M ion dictates solution pH during cluster formation, crystallization kinetics, crystal yield, and tunable optical properties. Time-resolved small-angle X-ray scattering (SAXS) and 27Al magic-angle spinning (MAS) nuclear magnetic resonance (NMR) unveil the partial decomposition of aluminate precursors and the synchronized self-assembly of M@Th12@L8. This work advances our understanding of thorium hydrolysis in heterometallic systems and establishes a modular strategy to prepare MOCs with tailored architectures and functionalities.
Composite solid electrolytes are the most promising candidates for next-generation commercial electrolytes in Li metal batteries. However, the inevitable layered-structure caused by the agglomeration or sedimentation severely impairs the stability and ion conductivity. In this work, by using the phase-inversion within 20 s, we successfully uniformly dispersed Li6.5La3Zr1.5Ta0.5O12 (LLZTO) nano-powders into cellulose acetate, generating a highly conductive and stable 3D composite skeleton film with the thickness of 50 µm. Due to the high heating/cooling rate of 104 ℃/min, the ultrafast high-temperature sintering (UHS) enables the LLZTO powders with high crystallinity and a size of ~500 nm. Filling the PEGDA polymer, the resulting composite electrolyte films exhibit an ion conductivity of 1.2 mS/cm, nearly 6 times that of the electrolyte film without LLZTO. The composite electrolyte films exhibit excellent stability with Li metal, resulting in a reversible cycling over 2200 h at 0.2 mA/cm2. Using LiFePO4 and Li metal, the full cell shows a high capacity retention of 99.6% after 200 cycles and a high rate performance of 1 C. Pairing with NCM811, the cell stable cycles over 110 cycles with a Coulombic efficiency of 99.2%. This work provides a novel strategy for designing high-performance composite solid electrolytes and paves the way for developing practical SSLMBs with enhanced safety, high energy density, and long cycle life.
Olivine-type LiMnxFe1-xPO4 (LMFP) cathode materials with high energy density (≈700 Wh/kg) and high discharge platform (4.1 V vs. Li+/Li), have attracted considerable interest and prominence in the realm of lithium-ion batteries (LIBs). Nevertheless, the cycling stability of LMFP highly associated with electrolyte compatibility, which suffers from the subsistent transition-metal dissolution under hydrofluoric acid (HF) corrosion and unstable interface formation, posing significant challenges. Herein, we demonstrate that a multifunctional electrolyte additive, (Trimethylsilyl)methyl acetate (TMSA), possesses the good compatibility with LiMn0.60Fe0.40PO4 cathode material. Its features are embodied in the HF elimination, proton coordination and hierarchic cathode electrolyte interface (CEI) formation to prevent electrolyte decomposition and swelling of conductive carbon layer inside materials. Therefore, the LiMn0.60Fe0.40PO4ǁLi batteries can sustain the significantly enhanced capacity retentions of 67.5% after 500 cycles at room temperature (25 ℃) and 74.4% after 400 cycles at high temperature of 55 ℃, even contributing to an improved specific capacity of 113.8 mAh/g at 15 C rate (vs. 88.1 mAh/g in the counterpart). Impressively, LiMn0.60Fe0.40PO4ǁgraphite pouch cell retains a 93.76% capacity after 300 cycles. These much better electrochemical performances from the facile yet available design of electrolyte additive shows the great importance and potential for the developments of LiMn0.60Fe0.40PO4-based LIBs.
The orbital differentiation of transition metal ions demonstrates a critical role in modulating the structure and properties of two-dimensional π-d conjugated metal-organic frameworks (2D c-MOFs), which is possible to achieve the high-capacity and high-voltage features in rechargeable metal-ion batteries. Herein, we propose and demonstrate the strategy of coordination chemistry with different transition metal ions to construct metal phthalocyanine-based 2D c-MOFs (NiPc-8O-Cu, NiPc-8O-Ni and CuPc-8O-Cu) with different central and peripheral metal-coordination redox-active sites, which were discussed for the first time as the advanced cathode materials for potassium-ion batteries (PIBs). Benefiting from the low-spin state and the closed-shell d-orbital of central metal, NiPc-8O-Cu has higher electron/ion conductivity and stronger electron delocalization, demonstrating fascinating electrochemical performance, including a high reversible specific capacity (194 mAh/g at 0.2 A/g) and a well long-term cycling performance (over 3000 cycles at 5.0 A/g). It is worth noting that NiPc-8O-Cu can also showcase the good cycle performance at wide-temperature (−20~60 ℃). These findings provide a general guideline for the development of high-performance 2D c-MOFs as electrode materials for metal-ion batteries by engineering "inside and outside" active-site strategy.
Solid polymer electrolytes present transformative potential for all-solid-state sodium metal batteries (ASSMBs) owing to their molecular tailorability, cost-effectiveness and ease of processability, yet face critical challenges including sluggish Na+ diffusion kinetics at room temperature, high-voltage oxidation tendency, and uncontrolled Na dendrite growth. To address these limitations, we propose an anion-regulation strategy through a hierarchically engineered composite polymer electrolyte (CPE) that strategically integrates (1) a high-concentration NaTFSI− optimized polyethylene oxide (PEO) matrix (EO: Na+ = 6:1) and (2) a mechanically reinforced polyacrylonitrile (PAN) scaffold embedded with uniformly dispersed UIO-66 metal–organic framework nanoparticles (UIO-66@PAN). High-concentration TFSI− dissociation activates mobile anion-Na+ cluster species that form dynamic percolation networks, establishing low-energy-barrier pathways for accelerated Na+ migration (1.01 mS/cm at 30 ℃). Meanwhile, the UIO-66@PAN scaffold delivers exceptional tensile resilience (3.46 MPa) for the CPE membrane, meanwhile sub-nanometer precision of porous architecture (7.5–8.1 Å in UIO-66 vs. 7.9 Å for TFSI−) enables steric-electronic dual-anchoring effects for TFSI− immobilization, achieving a high Na+ transference number (tNa+ = 0.76). In a solvent-free, layer-stacked ASSMB assembly with sodium vanadium phosphate (NVP) cathode (1 mAh/cm2), 25 µm CPE and the Na foil, the prototype achieves 91.3% capacity retention over 200 cycles at room temperature, rate behavior up to 1 C as well as robust cyclability across a wide temperature range (25–80 ℃). This molecular-scale engineering of anion behavior in the CPE design thus establishes a new paradigm for the practical ASSMB prototyping.
A facile ammonium salt-mediated double-deck stacking strategy is first put forward to fabricate Li3YCl6 (LYC) halide solid electrolyte (HSE), which capitalizes on the dual functionality of NH4Cl in terms of dehydration and chlorination. It is worth mentioning that the obtained LYC features nanoparticles (< 400 nm) and demonstrates an excellent ionic conductivity of 2.33 × 10–4 S/cm at 25 ℃. In addition, the integration of LYC into all-solid-state cell with LiCoO2 cathode and Li anode delivers a high initial discharge specific capacity of 139.5 mAh/g at 0.1 C with a capacity retention ratio of 87.7% after 50 cycles. Encouragingly, the well-designed strategy not only enables the adoption of low-cost metal oxides and hydrates as raw materials, but also realizes the regeneration of damp LYC HSE. Hence, these encouraging results manifest that the proposed synthesis strategy delivers extremely economic benefits and valuable insights for developing HSEs.
In response to the increasing societal demand for efficient power and energy storage solutions, the development of novel battery technologies to complement existing lithium-ion batteries (LIBs) has emerged as a pivotal area of research. Sodium-ion batteries (SIBs), owing to the similarities in the physicochemical properties of sodium and lithium, have interpreted as promising candidates for next-generation secondary batteries. However, current research predominantly concentrates on the optimization of cathode and anode materials, as well as electrolytes, with insufficient attention paid to the critical role of inactive materials, such as binders, conductive agents, and separators. While electrode and electrolyte materials are undeniably crucial in determining the electrochemical behavior of batteries, the presence of these inactive components exerts a significant influence on factors including cost, performance and safety. This review aims to offer a comprehensive overview of the development, classification, and challenges associated with these key inactive components, with particular focus on cross-material synergies on battery performance. It is anticipated that this review will provide valuable insights to facilitate the enhancement of SIB performance and contribute to the optimization of battery systems as a whole.
Achieving optimal reactive oxygen species (ROS) production requires carefully balancing these interactions to maximize therapeutic efficacy. Herein, we have successfully developed a nanosystem through defect substitution using CuCoFe-layered double hydroxides (LDHs) as a template, followed by Pt reduction on the layer, the resulting nanoalloy, denoted as CuPt alloy@LDHs, demonstrating remarkable ROS production activity. This superior ROS production was attributed to its low Gibbs free energy barrier for generating hydroxyl radical (·OH), as confirmed by both characterizations and density functional theory (DFT) calculations. Additionally, the nanoalloy exhibits good (NOx)-like activity, effectively disrupting the intracellular NADH/NAD+ cycling balance and enabling self-cycling of endogenous H2O2. This work highlights that CuPt alloy@LDHs can effectively disrupt the redox homeostasis in tumor regions, significantly improving therapeutic efficacy and overcoming the limitations of current nanoalloy catalytic therapies.
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