Physics
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ABSTRACT Nanofiltration (NF) membranes are highly promising for selective lithium recovery from brines, yet their efficiency is significantly hindered by concentration polarization (CP) and membrane fouling. In this study, polyethyleneimine (PEI)‐based NF membranes functionalized with “liquid‐like” surfaces were developed via the covalent grafting of highly flexible molecular chains. These surfaces are demonstrated to induce an interfacial slip effect with a significantly increased slip length, which enhances cross‐flow velocity and effectively mitigates CP resistance. Meanwhile, the dynamic behavior of the flexible chains inhibits contaminant deposition, endowing the membranes with superior antifouling properties. Coupled with the enhanced chlorine resistance of the liquid‐like surfaces, stable separation performance was maintained throughout a 12‐day continuous operation test. The hydrophilic NH 2 ‐PEG‐functionalized membrane delivers a higher permeance of 21.7 L·m −2 ·h −1 ·bar −1 , along with an exceptional Mg/Li selectivity ( S Mg/Li = 67.8). The hydrophobic NH 2 ‐PDMS‐functionalized membrane achieves an even higher S Mg/Li of 88.5 while maintaining a permeance of 10.9 L·m −2 ·h −1 ·bar −1 . Both membranes maintain excellent Mg 2+ rejection, particularly under high‐salinity conditions. This work provides a versatile strategy for designing high‐performance membranes for sustainable lithium resource recovery.
ABSTRACT Ammonium ions (NH 4 + ) offer a dual mechanism for electrochemical storage, combining tetrahedral geometry for hydrogen bonding with a non‐polar π‐face primed for cation–π interactions. However, no single electrode material has successfully harnessed both pathways synergistically. Herein, ZnCo‐ZIF/N‐MXene heterostructure engineered as a molecular cation trap deliberately integrating complementary chemisorption sites. The conductive N‐MXene scaffold provides abundant hydrogen‐bonding acceptors, while the anchored ZIF nanoparticles, electronically modulated by interfacial charge transfer, activate robust cation–π interactions via π–d orbital hybridization at Co centers. This dual‐reaction‐center mechanism enables unparalleled NH 4 + storage, delivering an ultrahigh specific capacitance of 1380.6 F g −1 at 1 A g −1 with 94.3% capacitance retention over 10 000 cycles. A suite of in/ex situ spectroscopic and electrochemical probes, including XAFS and in situ EIS, provides direct evidence for the charge transfer that enables cation–π bonding and the highly reversible kinetics afforded by cooperative hydrogen bonding. Constructed as a full‐cell NH 4 + ‐HSC (ZIF/N‐MXene//ZIF‐rGO), the device achieves a top‐tier energy density of 98.2 Wh kg −1 at 1000 W kg −1 , with 88.3% capacity retention over 10 000 cycles—significantly outperforming state‐of‐the‐art systems. This work establishes a definitive interface‐engineering strategy for harnessing molecular‐ion duality, paving the way for next‐generation energy storage systems.
ABSTRACT Circularly polarized light (CPL) provides additional degrees of freedom for visual information processing in artificial photonic synapses (APS). However, achieving carrier dynamics modulation for synaptic behavior conflicts with maintaining the inherent chiral properties of the material. Here, we propose an anion‐mediated carrier relaxation strategy to achieve CPL perception and synaptic functional coupling in the chiral perovskite material. The partial substitution of I − with SCN − in the chiral perovskite (R/S‐NEA)PbI 3 lattice reduces the migration barrier of I − , facilitating iodine vacancy generation and inducing intermediate energy level formation. These intermediate states extend carrier relaxation times, while the similar ionic radius of SCN − and I − maintain the intrinsic chiral optical properties of the material. The CPL‐sensitive APS was prepared using this modified chiral material. Leveraging polarization‐dependent temporal dynamics of APS, a multidimensional neuromorphic vision system integrating CPL information, parallax, and optical flow features was constructed for 3D motion analysis. In 3D scene testing, the system achieves a fish trajectory tracking accuracy of 97.25% and reliably distinguishes six distinct motion directions. This approach provides a promising pathway toward intelligent visual perception systems to achieve efficient information processing in complex application scenarios, such as autonomous driving and robotics.
ABSTRACT The large‐scale application of aqueous zinc‐ion batteries (AZIBs) is impeded by critical challenges, including uncontrolled zinc dendrite growth, severe parasitic side reactions, and hydrogen evolution reaction. To address these issues, we introduce a versatile diprotic acid, malonic acid (Mal), as a functional electrolyte additive. Combined experimental and theoretical results, we propose a new “etching‐adsorption‐deposition” mechanism, where Mal and its protons synergistically form a dendrite‐free, (101)‐oriented Zn anode. Concurrently, Mal participates in the Zn 2+ solvation sheath, effectively inhibiting water activity and hydrogen evolution reaction. These synergistic effects endow it with outstanding electrochemical stability, the Zn//Zn cell exhibits ultra‐long cycle stability over 4700 h at 5 mA cm −2 and 1 mAh cm −2 . Furthermore, the Zn//Cu cell delivers a significantly improved reversibility with an average Coulombic efficiency (CE) of 99.86% after 2000 cycles at 5 mA cm −2 and 1 mAh cm −2 . Surprisingly, Mal molecules exhibit a strong affinity for the V 2 O 5 cathode, forming a protective layer that mitigates vanadium dissolution and suppresses parasitic by‐products. The Zn//V 2 O 5 full cell consequently demonstrates excellent cycling performance, with 98.25% capacity retention after 1000 cycles at 1 A g −1 . Notably, its stability extends to extreme conditions, as it also maintains 64.5% capacity retention after 5000 cycles at 10 A g −1 .
ABSTRACT Electrocatalytic nitrate reduction reaction (NO 3 RR) towards ammonia (NH 3 ) production is a critical process that sustainably converts hazardous nitrate to value‐added chemicals. Amorphous metal‐based nanomaterials are promising NO 3 RR catalysts owing to the abundant surface active sites, but their performance is still unsatisfactory for practical needs. We develop a robust one‐pot strategy to prepare a family of amorphous PdMP ( a ‐PdMP, M = Cu, Ni, Co, Fe, Mn, and Zn) nanoparticles with high yield, high structural stability, uniform morphology, and tunable composition. Impressively, the as‐prepared a ‐PdCoP nanoparticles show excellent electrocatalytic activity (onset potential measured at +0.3 V vs. reversed hydrogen electrode), high NH 3 selectivity, and outstanding long‐term stability (Faradaic efficiency (FE) maintained > ∼98% at 200 mA cm −2 for 200 h) in NO 3 RR. Theoretical calculations demonstrate that alloying in PdM can enhance overall electron exchange/transfer, while phosphization helps to stabilize the metal valence. Particularly, the a ‐PdCoP possesses a moderate d‐band center to avoid intermediate overbinding, meanwhile, it has the lowest work function to accelerate the electron transfer during NO 3 RR. Our work demonstrates that synergistic amorphization and phosphization of Pd alloy nanocatalysts can greatly promote their activity and durability in NO 3 RR. The universal synthesis approach provides guidance to prepare amorphous multielement nanomaterials as highly efficient electrocatalysts.
ABSTRACT Lithium‐sulfur (Li‐S) batteries have attracted considerable attention as high‐energy storage systems, but are hindered by sluggish lithium polysulfide (LiPSs) redox kinetics and the shuttle effect. Although heterostructured catalysts can alleviate these issues by tailoring interfacial electronic structures, it remains difficult to precisely control the interfacial composition during synthesis, and the stepwise LiPSs conversion mechanism at such interfaces is not fully understood. Herein, we propose a facile synthesis strategy based on thermodynamic modulation for the directional growth of MoNi x /Mo 2 C heterostructures and elucidate their catalytic mechanism in Li‐S batteries. By tuning the Ni/Mo precursor mass ratio, a continuous and controllable evolution from a MoNi x solid solution to a MoNi x /Mo 2 C heterostructure is achieved, with MoNi x /Mo 2 C‐NCNFs exhibiting the optimal catalytic effect on LiPSs conversion. An initial discharge capacity as high as 1343.9 mAh g − 1 at 0.2 C was achieved with the MoNi x /Mo 2 C‐NCNFs separator. Combined experimental and theoretical analyses reveal that the charge redistribution induced at the heterointerface leads to an upward shift of the d‐band center, activating a “functional zoning and tandem catalysis” mechanism in which the phases and interface cooperatively accelerate stepwise LiPSs conversion. These findings clarify how interfacial electronic structures govern LiPSs conversion and provide practical guidelines for high‐performance catalysts.
Topological defects determine the collective properties of anisotropic materials. Nonetheless, it is not fully understood how their configurations are controlled, especially in three dimensions. In living matter, contributions of two-dimensional topological defects to biological functions have been demonstrated, but whether three-dimensional polar defects have any biological relevance is unclear. Here we report a charge-preserving transition between three-dimensional defect configurations driven by boundary geometry and independent of material parameters. Moreover, we find that three-dimensional polar defects in the mouse embryo are the sites where fluid-filled lumina form, essential structures for subsequent development. We validate these findings by experimentally perturbing embryo shape beyond the transition point, which results in the creation of additional lumen initiation sites near predicted defect locations. Overall, our results reveal how boundary geometry controls polar defects, and how embryos use this mechanism for shape-dependent lumen formation. We expect this defect-control principle to apply broadly to systems with orientational order.
ABSTRACT High‐entropy transition metal sulfides (HESs) exhibit great potential as anodes for sodium‐ion batteries owing to their synergistic entropy stabilization, lattice distortion and cocktail effects. However, potential phase separation caused by multi‐component incompatibility severely limits their performance. Herein, we propose a low‐mixing‐enthalpy strategy through regulation of element chemical compatibility to precisely design high‐performance HES anodes. This strategy enables the successful synthesis of a single‐phase Co‐Fe‐Ni‐Mn‐Cr HES solid solution (HES‐Cr). In contrast, inferior compatibility among components in Co‐Fe‐Ni‐Mn‐Mo HES (HES‐Mo) leads to its phase separation. The electron delocalization in HES‐Cr enhances conductivity and metal‐sulfur bond covalency, while moderate lattice distortion alleviates volume changes and stress concentration during Na + insertion/extraction and lowers the Na + migration barrier. Consequently, the HES‐Cr delivers excellent Na + storage performance, including a high reversible capacity of 845.2 mAh g −1 at 0.2 A g −1 and ultra‐high rate property of 497.5 mAh g −1 even at 40.0 A g −1 along with long stability, outperforming HES‐Mo and most HES‐based anodes. Furthermore, we propose a three‐parameter descriptor to predict single‐phase high‐entropy materials across a broader compositional range. This work provides a new approach for rational design of single‐phase HESs and deepens understanding of their composition‐phase‐performance relationships.
conductivity, excellent compatibility with cathodes, and good mechanical deformability. However, many of these conductors exhibit chemical and electrochemical instability when in contact with the reductive anodes, which hinders the direct use of lithium metal as anodes with extraordinarily high specific capacities and limits the overall energy density of halide-based ASSLBs. Therefore, enhancing the anode compatibility of halide SSEs has become a critical task in ASSLB development and has attracted broad research interest. Herein, the underlying mechanisms responsible for the instability of halide SSEs against the lithium anode are elucidated based on both experimental observations and theoretical calculations. Recent strategies and progress aimed at improving the compatibility of halide SSEs with lithium anodes are summarized. Moreover, the effects of pressure and volume changes on the interfacial compatibility between halide SSE and lithium metal are discussed. In addition, the current challenges and future research directions are analyzed, aiming to provide theoretical insights and guidance to support further advancements in Li-M-X type solid-state electrolytes and all-solid-state lithium batteries.
The quantum spin Hall (QSH) effect represents a prototypical 2D topological phase in which time-reversal symmetry protects dissipationless, spin-polarized helical edge states coexisting with an insulating bulk. Owing to its magnetic-field-free operation, intrinsic spin-momentum locking, and electrically tunable topology, the QSH state has long been regarded as a promising platform for ultra-low-power, ultra-fast electronics, spintronics, and topological quantum computation. Despite this compelling vision, experimental realizations of QSH-based functionalities remain confined to a limited number of material systems and device geometries, typically operating at cryogenic temperatures and over restricted length scales. In this Perspective, we critically reassess the field by synthesizing the central promises of the QSH effect and analyzing the intrinsic material limitations and extrinsic functional bottlenecks that have hindered its technological translation. We argue that future progress will depend not only on the discovery of novel QSH materials but also on the engineering of topological functionality through large-gap systems, chemically robust platforms, and interaction- or proximity-induced phases. Viewed from this perspective, the QSH effect emerges not as a stalled technology, but as a foundational framework for designing next-generation electronic, spintronic, and quantum devices.
Polyurethane is indispensable to our life, but its end-of-life wastes bring severe environmental problems due to the bulky volume and thermoset nature. The regenerated products based on current recycling strategies normally have fixed mechanical properties, limiting adaptability to diverse applications. Here, we present a chemical recycling strategy that can transform polyurethane waste into smart materials with end-user-on-demand programmable properties and adaptable applications. It is achieved through inserting a thermal-triggered network topology transformation switch in the polyurethane. The network topology transformation switch endows the regenerated materials with on-demand mechanical programmability, which could achieve a 54-fold modulus enhancement from 5 MPa (soft rubber) to 270 MPa (rigid/semi-rigid plastic). More importantly, the thermal-triggered feature empowers end-users not only to tailor material stiffness post-production, but also to benefit from enhanced portability, functional adaptability for multi-scenario applications. Our strategy of recycling waste into products with programmable properties and adaptable applications is not only environmentally friendly but also highly appealing to the end-users, providing a promising direction in the future reuse of plastic waste.
Self-healing polymers governed by supramolecular and dynamic covalent interactions are redefining structural design and functional integration in contemporary materials. Reversible supramolecular motifs, including hydrogen bonding and electrostatic interactions, enable rapid interfacial reconstruction and damage tolerance, whereas dynamic covalent bonds, such as Diels-Alder, disulfides, provide mechanically robust, reconfigurable, and recyclable network architectures. Their synergistic integration yields materials with repeatable healing, robust mechanics, and multimodal responsiveness. These advances have accelerated progress in flexible electronics, particularly capacitive sensing, where dedicated multilayer architectures, printable conductors, and minimal conductive dopants deliver enhanced sensitivity, a broad operational window, and rapid electrical and mechanical recovery; however, challenges such as scalable processing and property reconciliation remain unresolved. This review highlights recent advances in multifunctional dynamic polymer networks by delineating supramolecular and dynamic covalent self-healing behaviors, their synergistic coupling, and their deployment in state-of-the-art self-healing sensor devices, providing insights for high-performance flexible sensing technologies.
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