As a kind of promising energy storage devices with the potential advantages of high levels of safety, costeffectiveness, and environmental sustainability, aqueous supercapacitors have received extensive attention recently. Constrained by the limited voltage window of water in aqueous electrolytes, improving the energy density that is the main shortcoming for supercapacitors mainly relies on the increase of the specific capacitance of the electrodes. Herein, we report an electrode with a high areal capacitance of 16.96 F cm- 2 at 1 mA cm- 2 that consists of the hydrothermally grown MnCo2O4 and the subsequently electrochemically deposited NiCoP, i.e., MCO/NCP, on Ni foam. 90.2% of the original capacitance can be maintained after 8000 cycles at 50 mA cm- 2, with nearly 100% coulombic efficiency during cycling. The asymmetric supercapacitor assembled with the MCO/ NCP cathode and active carbon anode tested in 2 Mol L- 1 KOH aqueous electrolyte, delivers a leading energy density of 0.793 mWh cm- 2 at 0.800 mW cm- 2 and notable cycling performance with 80.0% capacitance retention and 100% coulombic efficiency over 15,000 cycles at 50 mA cm-2
Carbon-based hole-transport-layer (HTL)-free CsPbI2Br solar cells present a promising balance among efficiency, stability and cost. Nevertheless, their performance is still restricted by bulk and interfacial defects, as well as energy level mismatch between CsPbI2Br and its neighboring layers. Herein, a series of uracil-based additives, including uracil, 5-cyanouracil (5-CU) and 5-nitrouracil (5-NU), are introduced into CsPbI2Br to construct dipolar molecular bridges that can simultaneously passivate defects (i.e., uncoordinated Pb2+ and mobile halide ions in CsPbI2Br and uncoordinated Sn4+ on the surface of SnO2), improve crystallinity, and regulate interfacial energy level alignment. It is further found that the most polar 5-NU exhibits the best ability to realize these functions. The 5-NU-optimized device thus achieves a leading power conversion efficiency of 16.10%, with an exceptional open-circuit voltage of 1.345 V, significantly reduced hysteresis and excellent operational stability.
The Co 3 O 4 @NiFe LDH-3 heterostructure shows excellent activity with ultralow overpotentials ( η 10 = 167 mV, η 1000 = 222 mV) and stability over 1000 h, owing to interfacial synergy that activates the LOM, while Co 3 O 4 stabilizes active NiOOH species.
Developing low-cost, high efficient, and durable non-precious metal electrocatalysts for is for the oxygen evolution reaction (OER) is pivotal for advancing sustainable water electrolysis toward commercial hydrogen production. Herein, CoSe2@NiSe2/NF heterostructured electrocatalysts were prepared on three-dimensional nickel foam (NF) substrate by facile solution selenization combined with hydrothermal method. The as-prepared catalyst with heterostructure and interconnected flake-like structures optimizes OH- intermediate adsorption and accelerates charge transfer at the CoSe2/NiSe2 interfaces, exposes abundant active sites to facilitate mass transport and electrochemical reactions, then boosts the OER performance. Electrochemical measurements demonstrate that the CoSe2@NiSe2/NF-2 catalyst exhibits an overpotential of 229 mV, a Tafel slope of 43.1 mV/ dec, and stable operation for 100 h at 10 mA/cm2. Notably, it maintains exceptional durability under industrialrelevant conditions, sustaining stable performance for 400 h at a high current density of 1 A/cm2. This work provides a new idea for constructing heterostructured electrocatalysts with optimized electronic structures and robust stability, offering promising insights for the design of high-performance OER catalysts toward practical water-splitting applications.
This study develops a high-performance flexible electrode for aqueous asymmetric supercapacitors (ASCs) by insitu growing interconnected CuCo-layered double hydroxide (CuCo-LDH) nanosheets on carbon cloth (CC) using ZIF-67 as a precursor, followed by NiCo2S4 (NCS) electrodeposition to form a hierarchical CuCo-LDH@NCS structure. The optimized electrode achieves exceptional areal capacitance of 11,400.0 mF cm- 2 (1 mA cm- 2) and superior cycling stability, maintaining at 8244.0 mF cm- 2 (30 mA cm- 2), with 86.4 % capacitance retention after 6000 cycles. The assembled ASC (CC@CuCo-LDH@NCS//AC in 2 M KOH) delivers high energy density of 0.614 mWh cm- 2 at power density of 0.800 mW cm- 2 and retains 89 % capacitance after 10,000 cycles (30 mA cm- 2). These results demonstrate outstanding energy density, cycling stability, and potential for flexible energy storage
Transition metal selenides, recognized for their high theoretical capacities, are considered attractive anode candidates for sodium-ion batteries (SIBs), yet their performance is often impeded by slow charge/ion transport and pronounced volume changes caused by repeated sodiation/desodiation. To address these issues, we herein report the rational synthesis of a freestanding three-dimensional membrane comprising CoSe2/FeSe2 heterojunction nanoparticles uniformly encapsulated within an interconnected carbon nanofiber network (denoted as CoSe2/FeSe2@CNFs). Theoretical and experimental results indicate that the abundant CoSe2/FeSe2 heterointerfaces facilitate interfacial charge redistribution and strengthen Na+ adsorption, synergistically boosting the reaction kinetics. Benefiting from these structural merits, the CoSe2/FeSe2@CNFs anode achieves outstanding sodium storage performance, retaining 349.1 mAh g–1 after 600 cycles at 2 A g–1 and preserving 288.5 mAh g–1 even after 2500 cycles under a high current density of 5 A g–1. Furthermore, the reversible conversion mechanism is directly elucidated through in-situ and ex-situ characterizations and analyses. This work not only demonstrates an effective heterostructure engineering strategy, but also offers a viable pathway toward developing high-performing binder-free anodes for advanced energy storage applications.
ABSTRACT The gravimetric and volumetric energy densities of 500 Wh kg –1 and 1000 Wh L –1 are considered as the “holy grail” target values for the development of all‐solid‐state lithium pouch batteries. However, the substantial amount of non‐energy‐providing deformable catholytes in conventional catholyte‐based composite cathodes limits the theoretical values of the energy densities to approximately 400 Wh kg –1 and 900 Wh L –1 , respectively. Here, we propose a design strategy for catholyte‐free composite cathodes using deformable halide cathode for the replacement of the non‐energy‐providing catholyte to increase the energy density. Based on this strategy, the gravimetric and volumetric energy densities of all‐solid‐state lithium pouch batteries improve by an average of 30% and 11%, respectively. Compared with conventional catholyte‐based composite cathodes, the energy densities of these batteries now exceed 500 Wh kg –1 and 1000 Wh L –1 , respectively. The catholyte‐free composite cathode design is expected to facilitate the industrialization of high‐energy‐density all‐solid‐state lithium pouch batteries.
Supercapacitor diode (CAPode) is an emerging type of electrochemical logic device that integrates ions and electrons as the coinformation carriers, thus being a promising building block for constructing new-type iontronic circuits and achieving seamless brain-computer interaction. However, the lack of understanding on its basic process, i.e., nanoconfined ion transport, greatly blocks the further enhancement of its ion rectification capability and ion transport kinetics. Herein, on the basis of in-depth analysis of the host-guest interactions in the nanoconfined space, a nanoconfined water mediated strategy is proposed to manipulate the ion transport behaviors in typical layered materials, i.e., tungsten oxides (WO3·nH2O, n = 0, 1, 2). The results reveal that WO3·H2O presents an optimal ion rectification capability and superior ion transport kinetics, much outperforming those of WO3·2H2O or WO3 with more or less structural water. Consequently, the WO3·H2O-based CAPode delivers a record-high rectification ratio of 253, an ultrahigh response frequency of 549 Hz, and an excellent cycling stability of up to 5000 cycles, enabling it to handle various complex ion/electron-coupling logic operations. More attractively, WO3·H2O is demonstrated to possess superior biocompatibility, endowing the as-built CAPode with great potential in the cutting-edge field of brain-computer interactions.
Biomass-derived hard carbon is regarded as a promising anode material for sodium-ion batteries owing to its low cost, sustainability, and structural tunability. However, the interplay between carbonization temperature, microstructural evolution, and Na+ storage mechanism remains insufficiently understood. Herein, hard carbon materials were prepared from waste rubberwood by carbonization at 1100-1500 degrees C to systematically elucidate the structure-property relationship governing sodium storage behavior. Structural characterizations reveal that increasing carbonization temperature enhances graphitic ordering, decreases interlayer spacing, and reconstructs pore architecture and surface chemistry. Among all samples, HC-1300 achieves an optimal balance, featuring moderate graphitization, interconnected micro-mesoporous networks, and abundant C=O functional groups, which collectively facilitate rapid Na+ transport and high reversibility. As a result, HC-1300 delivers a high reversible capacity of 324.7 mAh g-1 with an initial Coulombic efficiency of 71.9% at 20 mA g-1, together with excellent rate capability and cycling stability. EIS, DRT, and GITT analyses confirm reduced charge-transfer resistance and enhanced Na+ diffusion kinetics. Furthermore, in situ X-ray diffraction reveals reversible (002) peak evolution without metallic Na formation, indicating a multistage sodium storage mechanism involving adsorption, intercalation, and pore filling. This work highlights the critical role of carbonization temperature in designing sustainable hard carbon anodes for sodium-ion batteries.
Room-temperature sodium-sulfur (RT Na-S) batteries face critical challenges from polysulfide shuttling effects and sluggish redox kinetics, requiring an optimal balance between adsorption and catalysis as dictated by the Sabatier principle. Herein, we designed a carbon-supported ruthenium (C-Ru) structure with interfacial electronic coupling to resolve this adsorption-catalysis conundrum. Comprehensive density functional theory (DFT) calculations were first conducted to investigate the atomic-level impact of the C-Ru composite on polysulfide conversion. The substantial charge transfer from Ru to carbon optimally tunes polysulfide adsorption, facilitating sulfur redox kinetics while dramatically lowering the Na2S decomposition barrier. Geometric and electronic analyses confirm that interfacial charge redistribution systematically weakens Na─S bonds. Guided by these insights, we designed a sponge-like porous carbon-Ru nanocomposite as sulfur host (SPC-Ru) with exceptional electrochemical performance: 924.3 mAh g- 1 after 100 cycles at 0.2 A g- 1 and ultralow capacity decay of 0.097% per cycle over 500 cycles at 2 A g- 1. This work establishes interfacial electronic coupling as an effective strategy to reconcile adsorption-catalysis conflicts in metal-sulfur batteries, offering a rational pathway toward high-energy-density and long-lifespan RT Na-S energy storage systems.
Abstract Garnet-based all-solid-state Li-metal batteries (ASSLBs) have garnered considerable attention due to their potential for high energy density. However, they remain severely plagued by short-circuit failures caused by Li dendrites penetration. Reducing voids that provide growth sites for Li dendrites within garnet-type solid-state electrolytes (SSEs, Li6.4La3Zr1.4Ta0.6O12 (LLZTO)) is one promising strategy. Furthermore, the sacrificial powder with identical composition required in conventional sintering processes contains La and necessitates synthesis, resulting in resource wastage. To overcome this limitation, we propose using Li2O as a sacrificial powder to enhance the densification of garnet-type SSEs, without containing La or requiring synthesis. With an appropriate Li2O dosage, the garnet-type SSEs can attain a relative density of up to 98.6% and a critical current density of 0.9 mA cm−2. LiFePO4/LLZTO/Li cells showcase an average discharge capacity of 145.4 mAh g–1 at 0.5 C and a capacity retention of 103.4% after 100 cycles at 0.2 C.
The rational design of conversion-kinetics-promoting framework architectures offers a powerful strategy to overcome the polysulfide shuttling and sluggish conversion kinetics that limit lithium-sulfur (Li-S) batteries. Here, we report a new covalent organic framework, TUS-44, constructed from tetrathiafulvalene-based 4,4',4'',4'''-([2,2'-bi(1,3-dithiolylidene)]-4,4',5,5'-tetrayl)tetraaniline and benzo[18]crown-6-derived 4,4',4'',4'''-(6,7,9,10,17,18,20,21-octahydrodibenzo[b,k][1,4,7,10,13,16]hexaoxacyclooctadecine-2,3,13,14-tetrayl) tetrabenzaldehyde linkers. The resulting imine-linked, π-conjugated framework integrates heteroatom-rich coordination sites within an electron-delocalized π-conjugated backbone, establishing a hierarchical, site-specific interaction network (N > O > S) that governs Li+ coordination, polysulfide anchoring, and dynamic charge redistribution. When coupled with conductive graphene to form an interfacial TUS-44@G architecture, the hybrid layer functions as a chemisorptive, conversion-kinetics-promoting interface that regulates soluble polysulfides, facilitates interfacial charge-transfer, and stabilizes intermediate species throughout cycling. This synergistic chemical-electronic coupling yields remarkable electrochemical performance: a high reversible capacity of 1455.7 mA h g-1 at 0.2 A g-1, excellent rate capability of 773 mA h g-1 at 10 A g-1, and outstanding durability with 0.034% capacity fading per cycle over 1000 cycles at 5 A g-1. A Li-S pouch cell incorporating TUS-44@G further delivers an outstanding initial energy density of ∼674 Wh kg-1 at 0.05 A g-1 (sulfur loading 44.558 mg), underscoring the practical potential of architecting conversion-catalytic framework interfaces for high-energy, durable Li-S batteries.
The Mach band effect enhances luminance boundary contrast, enabling biological vision systems to encode edge features while suppressing redundant information. This mechanism offers a pathway for information compression and energy-efficient computation in artificial vision systems. Hardware implementation faces challenges due to the complexity of neuronal ensembles and high power consumption. We propose a neuromorphic preprocessing architecture based on a monolithic iontronic memory device, where transient ion dynamics during abrupt electric field switching generates amplified currents to emulate dynamic Mach band enhancement. The device demonstrates sensitivity to high-slew-rate signals, achieving edge-sharpening amplification ranging from 4- to over 3,000-fold with increasing transition rates. This capability enables a broad operational frequency band (50 Hz–16 MHz), enhancing the signal-to-noise ratio in high-frequency regimes. For grayscale image edge extraction, this system achieves a data extraction rate of 0.649% while preserving the image contours.
Carbon‐based hole‐transport‐layer‐free CsPbI 2 Br solar cells are limited by high defect density and inefficient interfacial charge transfer. Herein, 5‐aminouracil (5‐AU) is introduced as a multifunctional additive to simultaneously regulate bulk defects and interfacial energetics. 5‐AU forms Pb–O coordination and hydrogen bonding, effectively suppressing defect states and nonradiative recombination. Meanwhile, during the film fabrication process, a subset of 5‐AU molecules can diffuse to the interface of the SnO 2 /CsPbI 2 Br, where they form molecular bridges that facilitate charge extraction and improve energy‐level alignment. As a result, the 5‐AU‐modified device achieves a power conversion efficiency of 15.63% with an exceptional open‐circuit voltage of 1.349 V, along with reduced hysteresis and significantly enhanced storage, thermal, and environmental stability.
In today's era of climate variability, severe electromagnetic pollution, and advanced infrared detection technology, multifunctional fabrics integrating personal thermal management (PTM), infrared stealth, and electromagnetic shielding capabilities have become crucial for human health and safety. In this work, we combine the inherently low infrared emissivity of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with the high electrical conductivity and strong solar light absorption properties of carbon nanotubes (CNTs) to achieve a multifunctional wearable fabric. This fabric has a low mid-infrared (MIR) emissivity of 0.33 in the 8-13 mu m band, thereby demonstrating remarkable infrared stealth properties and a passive radiative heating (PRH) performance of 3.1 degrees C, achieving an ideal covert thermal management effect. Its high electrical conductivity (4204 Sm(-1)) and solar light absorptivity (95.45%) have endowed it with satisfactory photo/electric-heating performance and an electromagnetic interference shielding efficiency (EMI SE) of 55 dB. Furthermore, this fabric also exhibits excellent self-cleaning properties, along with wearable characteristics that ordinary functional fabrics should possess, such as flexibility, washing resistance, and abrasion resistance. This work not only obtains a functional fabric with broad application prospects in various scenarios such as daily life and military steal, but also fully demonstrated that the conductive polymer PEDOT:PSS is expected to become a highly promising functional material in the fields of thermal regulation and camouflage.
Carbon-based hole-transport-layer-free CsPbI2Br solar cells have garnered significant attention due to their good stability and suitability as top cells in tandem devices. However, CsPbI2Br cells are prone to forming numerous defects, such as uncoordinated Pb2+ at grain boundaries during annealing, resulting in power conversion efficiency (PCE) of the corresponding photovoltaic devices far below their theoretical limit. To passivate defects in CsPbI2Br, molecular additives with different spatial conformations, including malononitrile (MDN), 1,3-dicyanobenzene (1,3-DCB), and 2,7-dicyanonaphthalene (2,7-DCN), are investigated. Theoretical calculations and experimental characterizations jointly demonstrate that, compared to alkyl-chain molecular frameworks, aromatic rings preferentially induce electron donation due to their pi-pi conjugation effect with terminal cyano groups (-CN). The pi-pi conjugation effect is more pronounced in naphthalene rings, enabling stronger passivation of uncoordinated Pb2+. Furthermore, the spatial distance between the two -CN in 1,3-DCB and 2,7-DCN molecules achieves an exquisite geometric matching with adjacent uncoordinated Pb2+ in the CsPbI2Br lattice. Thus, through the dual synergistic effects of electron donation and geometric matching, 2,7-DCN promotes the formation of a high-quality film with excellent crystallinity and low surface roughness. The champion PCE of the optimized device is enhanced from 11.80% for the control device to 15.87%, accompanied by a significant improvement in long-term stability.
In today’s era of climate variability, severe electromagnetic pollution, and advanced infrared detection technology, multifunctional fabrics integrating personal thermal management (PTM), infrared stealth, and electromagnetic shielding capabilities have become crucial for human health and safety. In this work, we combine the inherently low infrared emissivity of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with the high electrical conductivity and strong solar light absorption properties of carbon nanotubes (CNTs) to achieve a multifunctional wearable fabric. This fabric has a low mid-infrared (MIR) emissivity of 0.33 in the 8–13 μm band, thereby demonstrating remarkable infrared stealth properties and a passive radiative heating (PRH) performance of 3.1 °C, achieving an ideal covert thermal management effect. Its high electrical conductivity (4204 S·m−1) and solar light absorptivity (95.45%) have endowed it with satisfactory photo/electric-heating performance and an electromagnetic interference shielding efficiency (EMI SE) of 55 dB. Furthermore, this fabric also exhibits excellent self-cleaning properties, along with wearable characteristics that ordinary functional fabrics should possess, such as flexibility, washing resistance, and abrasion resistance. This work not only obtains a functional fabric with broad application prospects in various scenarios such as daily life and military steal, but also fully demonstrated that the conductive polymer PEDOT:PSS is expected to become a highly promising functional material in the fields of thermal regulation and camouflage.
Simultaneous compatibility of solid-state electrolytes (SSEs) with high-voltage cathodes and low-voltage anodes is crucial for high-energy-density all-solid-state lithium batteries (ASSLBs). However, deformable SSEs that integrate readily into ASSLBs rarely satisfy both requirements. Multilayer SSE membranes, such as halide SSEs paired with cathodes and sulfide SSEs with anodes, are therefore widely used but reduce energy density. Here, the low-cost, deformable oxyhalide-nitride SSEs, Li1.75+3xZrCl4.75O0.5Nx (0.1 ≤ x ≤ 0.3), are developed through dual-anion doping with O and N. The O and N incorporation preserves stability against the high-voltage LiCoO2 cathode while promoting a stable interface with the low-voltage Li13Si4 anode. A Li13Si4 | Li2.2ZrCl4.75O0.5N0.15 | Li13Si4 symmetric cell sustains stable plating/stripping for 2000 h with low overpotential. A Li13Si4 | Li2.2ZrCl4.75O0.5N0.15 | LiCoO2 cell using the oxyhalide-nitride SSE as a single membrane layer shows an initial specific discharge capacity of 134.72 mAh g-1 with 92.38% Coulombic efficiency and remains stable for 100 cycles.
Lithium-ion capacitors are promising candidates in future large-scale energy storage, but their practical application has long been restricted by the performance mismatches between the battery-type anode and capacitive cathode, especially the unsatisfactory charge storage capacity of the capacitive cathode. Herein, we demonstrate a novel capacitive cathode that is prepared by electrochemically dissociating a graphene-based highly compact porous carbon via anion intercalation chemistry. Comprehensive in situ characterizations reveal that under substantial electromigration forces, the anions in electrolyte can effectively intercalate into and dissociate the tightly stacked graphene nanosheets, thereby boosting the charge storage capacity. Remarkably, when used as the capacitive cathode of the lithium-ion capacitor, the activated material delivers an ultrahigh specific capacity of 390 mA h g-1 or 585 mA h cm-3, much outperforming those of state-of-the-art capacitive materials and even some advanced battery-type materials, thus taking a significant step in developing high-capacity capacitive cathode for applicable lithium-ion capacitors.
Carbon-cathode hole-transport-layer-free (HTL-free) CsPbI2Br solar cells offer a promising route toward high-performance-to-cost photovoltaics, yet their performance is largely constrained by defect-related losses. Here, a molecular strategy based on terpyridine derivatives is developed to regulate defect states, lattice distortion, and interfacial charge-transfer energetics in CsPbI2Br films. Owing to cooperative N/O coordination, [2,2':6',2″-terpyridine]-6,6″-dicarboxylic interacts with undercoordinated metal ions (Pb2+/Sn4+) and vacancy defect sites (I/O) at defect-rich surfaces, grain boundaries, and buried CsPbI2Br/SnO2 interfaces. This coordination-assisted regulation is associated with improved film crystallinity, reduced electronic non-uniformity, and more efficient interfacial charge extraction. As a result, carbon-cathode HTL-free CsPbI2Br devices achieve a leading comprehensive performance with a power conversion efficiency of 16.02%, minimal hysteresis, improved operational stability, and exceptional reproducibility. Furthermore, the applicability of this molecular approach is demonstrated in MAPbI3-based devices, highlighting its potential as a general strategy for defect regulation in the related optoelectronic devices.