Jingbin Han

Aqueous anion energy storage systems (AAEs) represent a promising class of energy technologies that combine high safety, environmental sustainability, and potential for green energy demands. In this work, low-cost NiMnCu-LDH is demonstrated for the first time as a high-performance cathode for AAEs based on Cl–/CO32– storage. As paired with the inexpensive hybrid anode of FeO(OH)/CNT and Bi2O2CO3 in a pouch battery, the AAEs deliver remarkable capacities at 25 and 0 °C, with ∼155 and ∼121 mAh g–1 at 300 mA g–1, respectively, sufficient to power light-emitting diode devices. Dynamic analysis illustrates mixed kinetics in concert: diffusion-controlled and pseudocapacitive processes. The cost-effectiveness of the AAEs derives from the scalable synthesis of both the NiMnCu-LDH cathode and hybrid anode. The outstanding battery performance is attributed to two-dimensional diffusion channels of LDH facilitating reversible intercalation/deintercalation of Cl–/CO32– within interlayers, along with valence transitions of Ni/Mn during charge/discharge cycles. The synergistic effects from mixed anions and the hybrid anode collectively enhance electrochemical performance, in which Cl– and FeO(OH)/CNT provide high capacity, while CO32– and Bi2O2CO3 stabilize cyclicality. These findings highlight the feasibility of the NiMnCu-LDH cathode coupled with the FeO(OH)/CNT and Bi2O2CO3 anode for AAEs to store Cl–/CO32–, offering research insights and development opportunities toward sustainable energy storage technologies.

Aqueous chloride-ion batteries (ACIBs) are promising energy-storage devices owing to environmental benignity, inherent safety, and abundant seawater electrolytes. However, their development is hindered by limited electrode choices and unsatisfactory electrochemical properties. Herein, we report high-performance ACIBs exploiting CoMnAl-LDH/CNT and BiOCl/CNT as cathode and anode in NaCl/NaOH aqueous electrolyte. CoMnAl-LDH/CNT exhibits a remarkable capacity of 114 mAh g–1 after 200 cycles at 200 mA g–1, with coulombic efficiency exceeding 98%. A specific capacity of 115 mAh g–1 is achieved at 400 mA g–1, with a voltage plateau around 0.8 V. Favorable performance is maintained at 0 °C, with a capacity of ∼142 mAh g–1 (∼89.1% of that at 25 °C). Over 2000 cycles, the capacity degradation per cycle is 0.025%, with lower decay of 0.013% in 200–2000 cycles, suggesting durable discharge capability. Enhanced Cl– storage is derived from fast two-dimensional ion-transport channels and topochemical transformation, facilitating reversible Cl– insertion/extraction and accommodating valence variations of Co/Mn. Interlayer water is crucial for ensuring structure and performance. Synergistic electrode design, electrolyte optimization, and CNTs/Al integration further boost electrochemical performance. This work establishes CoMnAl-LDH-based materials as feasible cathodes for reversible aqueous Cl– storage at 0 °C, highlighting great potential for future anion-shuttle batteries.

Membrane-based desalination is pivotal for addressing global water scarcity, with thin-film composite polyamide (PA) membranes as the industrial standard. However, thinning the PA selective layer to enhance permeability is hindered by rapid interfacial polymerization kinetics and uncontrolled monomer transport. Here, we introduce a scalable layered double hydroxide (LDH) nanosheet interlayer to precisely regulate PA formation. The LDH interlayer provides a uniform, hydrophilic platform that moderates amine diffusion via hydrogen-bonding, enabling the fabrication of an ultrathin (∼12 nm), continuous, and robust PA layer. The resulting LDH+PA membranes exhibit superior performance in both reverse osmosis and pervaporation. Notably, pervaporation desalination of 3.5 wt % NaCl achieved a water flux of 12.1 kg m–2 h–1 with a remarkable water/salt selectivity of 10362. This interlayer-mediated strategy offers a robust approach to controlling interfacial polymerization for high-efficiency desalination membranes.

Two‐dimensional (2D) transition‐metal compounds often suffer from the dissolution of active transition metals and structural collapse during electrochemical cycling. Herein, a sequential acid‐base regulation strategy is proposed to construct Zn and Al vacancies within layered double hydroxide (LDH) laminates, yielding a defect‐engineered NiZnFeAl‐V _Zn V _Al ‐Cl LDH. Benefiting from the synergistic effect of dual vacancies, LDH concurrently achieves “ion channel” and “ion locking” functionalities. The “ion channel” mechanism arises from vacancy‐induced disruption of the intrinsic c ‐axis transport barrier and the expansion of interlayer galleries into a three‐dimensional interconnected diffusion network, significantly enhancing Cl ⁻ diffusion. Meanwhile, the “ion locking” effect suppresses the Jahn–Teller distortion of Ni ³⁺ by strengthening metal‐oxygen bonds and inducing inherent local lattice distortions from cation defects, thereby preventing active‐metal dissolution and preserving structural integrity. Density functional theory (DFT) calculations further reveal that dual vacancies enhance the electronic density of states near the Fermi level, significantly improving conductivity and charge transfer efficiency. As a result, the NiZnFeAl‐V _Zn V _Al ‐Cl LDH delivers outstanding cycling stability, maintaining 99.8 mAh g ⁻¹ after 1950 cycles at 150 mA g ⁻¹ . This work provides comprehensive mechanistic insights into vacancy‐mediated performance enhancement in LDH and establishes a new perspective for exploiting defect chemistry in 2D materials toward advanced energy storage applications.

The rapid and efficient separation of nanoscale targets in liquid matrices presents a critical yet formidable challenge. Polyamide (PA) membranes, while recognized as the benchmark for industrial‐scale nanoscale separation, face ongoing limitations in performance optimization. Although advances in nanomaterials have enabled breakthroughs in PA membrane performance, scalable production remains hindered by integration challenges. Here, we present a scalable strategy to fabricate ultra‐thin (−2 h ⁻¹ bar ⁻¹ and a Na ₂ SO ₄ rejection rate of 95.7%, achieving one of the best‐reported levels. Leveraging the accessibility of LDH colloids and the scalable fabrication process, this strategy enables the production of large‐area membranes via spraying and IP, making it highly promising for purifying and recovering antibiotics.

Designing efficient, durable, and cost‐effective electrocatalysts for the oxygen evolution reaction (OER) remains a critical challenge in the development of advanced water‐splitting technologies. Herein, a series of CeO ₂ ‐decorated MgAl‐layered double hydroxide (LDH) heterostructures were rationally synthesized via a facile hydrothermal approach. Structural and morphological characterizations confirm the successful integration of CeO ₂ nanoparticles onto the LDH nanosheets without compromising the layered architecture. Among the synthesized catalysts, the C‐5L heterostructure exhibits superior OER performance in 1 M KOH, requiring an onset potential of 0.28 V and overpotential of only 0.32 V to deliver a current density of 10 mA cm ⁻² , significantly lower than its undoped and higher doped counterparts. The optimized catalyst also achieves the smallest Tafel slope (80 mV dec ⁻¹ ), the lowest charge‐transfer resistance (34 Ω), and the highest C _dl (4.21 mF cm ⁻² ), indicating enhanced reaction kinetics and increased electrochemically active surface area. Furthermore, it demonstrates the highest mass activity (28 A g ⁻¹ at 0.37 V vs. RHE) and exceptional operational stability over 100 h at 100 mA cm ⁻² . This study underscores the theme of interfacial engineering between CeO ₂ and LDH, providing valuable insights into designing high‐performance OER catalysts through controlled electronic coupling and defect modulation.

Fluoroarenes persist in aquatic environments because aromatic delocalization and aqueous speciation suppress selective C-F bond cleavage, limiting both reductive activation and direct hole oxidation. Hydroxyl radicals (·OH) can mineralize these contaminants, yet near-neutral·OH generation typically relies on added oxidants or Fenton chemistry, creating chemical demand and secondary residues. Here we report a carboxyl-functionalized crystalline perylene diimide photocatalyst (Carboxyl-PDI) that produces ·OH via a catalytic carboxyl-peroxyacid cycle under visible light. Carboxyl-PDI delivers a 50.94% apparent quantum yield for ·OH at 600 nm, achieves complete defluorination of 100 mg L⁻¹ perfluorophenol under AM1.5 G irradiation, and retains stable capacity for >500 h. Isotope labelling mass spectrometry and theoretical calculation identify a -COOOH intermediate and show hydrogen-bond gating to a neighbouring PDI carbonyl weakens the O-O bond by ~0.31 eV, enabling low-barrier homolysis for producing ·OH. A continuous-flow outdoor-sunlight reactor reaches 95.85% degradation, 90.67% defluorination and 79.68% mineralization, demonstrating scalable oxidant-free defluorination of perfluorophenol.

Aerogels, as highly efficient thermal insulation materials, exhibit significant potential for applications in building exterior insulation, power battery thermal protection, and aerospace thermal management. However, conventional polymer aerogels possess inherent limitations in thermal insulation performance, mechanical compressive strength, and flame-retardant safety, which impede their widespread engineering adoption. Herein, we propose a synergistic fabrication strategy integrating directional freezing and viscosity modulation. By precisely regulating the temperature gradient and incorporating layered double hydroxides (ZnMgAl-LDH) to tune the viscosity of hydrogel precursors, we enhanced the viscous resistance during ice crystal growth, thereby refining ice crystal dimensions. A honeycomb-like ZnMgAl-LDH/chitosan (CS) inorganic–organic hybrid aerogel with tunable pore size distribution was successfully constructed. The superlattice interface of ZnMgAl-LDH and the organic–inorganic hybrid interface synergistically reinforce phonon scattering (covering both long and short wavelengths), effectively suppressing solid thermal conduction and significantly improving the aerogel’s thermal insulation performance. Compared with pure CS aerogel, the hybrid aerogel with optimized pore size displays a lower thermal conductivity (0.03735–0.03936 W/(m·K)) and reduces the surface temperature by 6.9 °C under identical conditions. Moreover, the honeycomb microstructure endows the hybrid aerogel with excellent compressive resilience, retaining 72.4% stress after 50 compression cycles and achieving a compressive modulus 9 times higher than that of pure CS aerogel. Its flame-retardant performance is remarkably enhanced, with the limiting oxygen index (LOI) increasing from 21.5% to 41.4% (meeting high flame-retardant standards) and the peak heat release rate (PHRR) decreasing by 74.9%. Additionally, the hybrid aerogel exhibits superior hydrophobicity and environmental durability, highlighting its great potential for practical engineering applications.