The efficiency of carbon dioxide (CO2) adsorption in carbonaceous materials is primarily influenced by their microporosity and thermodynamic affinity for CO2. However, achieving optimal heteroatom doping and precise micropore engineering through advanced activation techniques remains a significant challenge. We introduce a solvent-free one-pot method using polythiophene, melamine, and KOH to prepare highly microporous, heteroatom-co-doped carbons (NSC). This approach leverages sulfur from polythiophene, nitrogen from melamine, and the activation agent KOH to enhance CO2 capture performance. Our results demonstrate that the optimized sample, NSC-800, achieves a CO2 adsorption capacity of 280.5 mg g–1 at 273 K and 1 bar, attributed to its high nitrogen (6.5 at.%) and sulfur (3.4 at.%) contents, a specific surface area of 2888 m2 g–1, and a micropore volume of 1.685 cm3 g–1. The moderate isosteric heat of adsorption (27.7 kJ mol–1) indicates a primarily physisorption-driven mechanism, as confirmed by close alignment with the pseudo-first-order polynomial model (R2 > 0.99) across temperatures of 303–323 K. This study reveals that NSC-800 also displays efficient regeneration after ten cycles of CO2 adsorption–desorption under flue gas conditions (15% CO2 and 85% N2 at 313 K), highlighting its potential as a regenerable, energy-efficient adsorbent for practical CO2 capture applications.
The present work reports on microscopic analyses of recombination at grain boundaries (GBs) in polycrystalline Li-doped (Ag,Cu)2ZnSn(S,Se)4 (Li-ACZTSSe) and Cu2ZnSnS4 (CZTS) absorber layers in high-efficiency solar cells (conversion efficiencies of 14.4% and 10.8%). Recombination velocities sGB were determined at a large number of GBs by evaluating profiles extracted from cathodoluminescence intensity distributions across GBs in these polycrystalline layers. In both Li-ACZTSSe and CZTS absorber layers, the sGB values exhibited wide ranges over several orders of magnitude with a median values of 680 and 1100 cm s–1 for the Li-ACZTSSe and CZTS absorbers. A model that provides a comprehensive explanation for this finding is presented and discussed in detail. Correspondingly, wide ranges for sGB can be explained by different positive or negative excess charge densities present at different GBs, leading to different downward or upward band bending on the order of several ±10 meV, provided that the net-doping density of the absorber layers is sufficiently large. As a result of the evaluation of the sGB, input parameters for multidimensional device simulations are obtained. It is revealed that the grain boundary lifetime closely matches the overall effective lifetime, indicating that grain boundary recombination is a key factor limiting the effective carrier lifetime of both Li-ACZTSSe and CZTS absorbers. The estimated VOC losses due to GBs reach up to 126 mV for Li-ACZTSSe and 88 mV for CZTS. This work highlights that reducing grain boundary recombination via improved passivation and increasing grain size is an effective strategy for achieving further efficiency improvements.
This study enhances quantum dot-sensitized solar cells (QDSSCs) with a photoanode containing gold and silver nanoparticles in a diamond-like carbon (DLC) matrix. The nanoparticles exhibit a synergistic effect, increasing the photoanode's response to visible light through localized surface plasmon resonance (LSPR). Simulations show that these nanoparticles improve charge transfer and cell efficiency by creating additional electron traps. DLC acts as a shield, protecting silver nanoparticles from corrosion, thus enhancing cell stability. The modified photoanode significantly increases the short-circuit current density compared to the standard photoanode, confirming the simulation results and demonstrating the potential for improved solar cell performance.
The advantages of the Ge–Pb-based perovskite solar cells (PSCs), such as low bandgap, have made this kind of PSC popular nowadays. Nevertheless, they have adverse properties that need to be fixed, such as short lifetime and fast crystallization process, which causes Ge defects. In this research, the passivation of Ge defects by using pyridinium chlorochromate methylamine iodine (PCCMAI) in the perovskite film (PF) structure is investigated. By using PCCMAI, the PSC's performance enhancement and surface morphology optimization were observed. It is determined that by the reaction of PCCMAI in the perovskite solvent, a coordination polydentate is formed in Ge–Pb mixed perovskite, and it results in the improvement of crystallization quality and electron transfer. After PCCMAI treatment of the Ge–Pb-based perovskite film, the measured power conversion efficiency (PCE) indicates that the performance of the fabricated PSC increased from 16.85% to 20.14%. Moreover, fabricated PSCs show an increment in stability after PCCMAI treatment.
In this study, lithium carbonate (Li2CO3) sourced from the Salar de Uyuni salt flat in Bolivia was used in the synthesis of cathode active material for Li-ion batteries. X-ray diffraction, atomic absorption spectrometry, and scanning electron microscopy analyses confirmed that the material had a high phase purity (99.59%, battery-grade) and a suitable morphology for active material synthesis, comparable to a similar commercially obtained material. Li[Ni1/3Mn1/3Co1/3]O2 (NMC111) was synthesized as a model system using Li2CO3 as the precursor and evaluated in full, large-format pouch cells along with three-electrode cells, using commercially relevant active material fractions and mass loadings for meaningful assessment of electrochemical performance. These cells exhibited capacities close to theoretical values and similar to that of commercially obtained NMC111, demonstrating the viability of the raw material. Operando X-ray diffraction analysis of aged pouch cells revealed that capacity loss was due to depletion of lithium inventory, without any disruption to the long-range cathode crystal structure or significant degradation in lithium kinetics. Postmortem analysis of the cycled electrodes further confirmed that transition metal dissolution and lithium trapping on the anode side were key contributors to the capacity fading observed in the pouch cells. This work demonstrates the potential of Salar de Uyuni's lithium resources for the production of cells relevant to practical applications.
Graphene aerogels (GAs) exhibit exceptional potential in energy storage, particularly for high-capacity supercapacitors (SCs), owing to their unique three-dimensional (3D) porous structure, high conductivity, and mechanical stability. Despite limitations in electron transport and surface polarity, their performance can be enhanced through structural optimization and synthesis strategies. This review traces the evolution of GAs from 1931 to 2024, integrating historical development with recent breakthroughs. It analyzes the synergistic effects of synthesis methods (self-assembly, template-assisted) and drying techniques (freezing/supercritical/ambient-pressure drying), elucidating structure–performance relationships and electrochemical mechanisms. This review also details the current research status of GAs applied in double-layer capacitors and pseudocapacitors. It identifies existing issues and summarizes ways to improve performance. Additionally, the research prospects of AI-assisted and in situ dynamic characterization in the development of GAs are outlined. In conclusion, this review aims to further advance high-performance GA electrode materials for SC applications and to anticipate future technological trends, providing a basis and academic reference for researchers in the energy storage field.
Uniform deposition is a promising strategy to inhibit dendrite growth and corrosion of the Zn anode in cost-effective energy storage systems: aqueous Zn-ion batteries (AZIBs). Herein, we report a regulating Zn2+ ions dissolution/deposition method for achieving a highly reversible Zn anode. 11-mercaptoundecanoic acid (MUA) as ligands was utilized to protect the (002) plane, benefiting from the strong affinity between the thiol group and Zn, with MUA anchoring in the form of Zn-S-RCOOH, which contributes to a stable interface for uniform deposition/deposition. More importantly, the MUA bonds to the (002) plane tightly and acts as a “rivet,” strengthening the Zn–Zn bonds of the (002) plane and leading to the high exposure of the (002) plane during the plating and stripping process. The MUA@Zn anode with 50 μm ultrathin thickness exhibits excellent stability (over 4000 h) and low overpotential at high current density (0.1–23 mA cm–2) and capacity (0.1–23 mAh cm–2). In addition, it also delivers a capacity of 194.1 mAh g–1 at 1 A g–1 and capacity retention of 95% after 1000 cycles. Consequently, our work provides a facial yet interfacial engineering approach in realizing the enhancement of Zn anode stability, exhibiting significant potential for practical application in AZIBs.
This study developed a symbiotic dual-confinement strategy integrating interstitial oxygen doping and carbon coating to enhance high-entropy alloys for high-current-density zinc-air batteries. Through the combination of theoretical cluster models with the experimental synthesis of MnFeCoNiCu@C high-entropy alloys, the synergistic suppression of demetalization and kinetic optimization was investigated. The dual-confined high-entropy alloys exhibited no significant attenuation for 1600 h in zinc-air batteries and resisted large current of 100 mA cm–2 impacts, with density functional theory calculations confirming lower d-band centers and higher formation energies, correlating with enhanced durability and reaction kinetics. This approach simultaneously addresses atomic-scale metal dissolution and nanoscale mass transfer limitations, surpassing conventional coating strategies. The findings establish a framework for designing robust high-entropy alloys, advancing their application in high-demand electrocatalysis and energy conversion technologies.
High-entropy oxides (HEOs) have sparked scientific interest recently as a potential material technology for lithium-sulfur (Li–S) batteries. This interest stems from their simultaneous roles as sulfur hosts and electrocatalysts, which provide enhancements to the performance of sulfur cathode composites. Nonetheless, their incorporation into the active material blend results in compromised energy density, particularly when their gravimetric proportion is substantial (≥10 wt.%, in the sulfur-based cathode). In this study, a manganese (Mn)-containing HEO (Sconfig ≥ 1.5R) was synthesized and subsequently coated onto a commercial Celgard separator at a low areal loading (~0.23 mg cm–2) with the aim of decreasing HEO content in the cathode composite material while still boosting lithium polysulfide (LPS) conversion kinetics. Li–S batteries incorporating this modified separator-high entropy oxide (MS-HEO) demonstrate exceptional electrochemical performance, achieving a high initial discharge capacity of ~1642 mAh g–1 at 0.1 C and a remarkably low-capacity fade rate of 0.055% per cycle over 450 cycles at 1 C. Remarkably, the MS-HEO batteries exhibited commendable electrochemical performance at high sulfur loading (~7 mg cm–2), delivering an initial discharge capacity of ~819 mAh g–1 during the first discharge and maintaining stable cycling up to 30 cycles at 0.1 C thereafter. Collectively, this work underscores the significance of precise adjustment of HEO compositions through low-temperature MOF calcination strategies and demonstrates their potential to enhance the electrochemical performance of Li–S batteries under the high-sulfur loading conditions necessary for future commercial applications.
Sb-Ge chalcogenides are known as effective phase change materials, making them ideal for optical data storage applications, detectors, and sensors. However, there have been no photovoltaic devices developed using these materials to date. In this work, Sb-Ge-Se crystalline thin films with different [Sb]/[Ge] atomic ratios are successfully grown for the first time through the selenization of co-evaporated Sb and Ge layers. The impact of the Se addition and temperature during the selenization process on the composition, structural, morphological, vibrational, and optical properties of the Sb-Ge-Se layers is investigated. The coexistence of Sb2Se3 and GeSe2 has been confirmed using various characterization techniques, including Grazing Incidence X-ray diffraction, Fourier Transform Infrared Spectroscopy, X-ray Photoelectron Spectroscopy and Raman spectroscopy. Additionally, Scanning Transmission Electron Microscopy has revealed Ge-enrichment regions surrounding the Sb2Se3 crystals. The composition of the co-evaporated film and final Ge content in the chalcogenide film govern the band gap energy, increasing from 1.41 to 1.83 eV. We present the inaugural operational SLG/Mo/Sb-Ge-Se/CdS/ZnO/ITO photovoltaic devices with a total efficiency of 1.34%. The primary factors limiting the device performance are the significant CdS diffusion into the active layer and the high defect density, as determined by Capacitance-Voltage and Drive-Level Capacitance Profiling. The devices exhibit excellent stability after 1 year of storage in ambient air. These first prototypes of Sb-Ge-Se crystalline thin films pave the way for advancement in the development of sustainable and stable photovoltaic devices.
High-entropy spinel oxides are promising anode materials for lithium-ion batteries owing to their unique crystal structures, which provide enhanced structural stability, multiple redox-active sites, and three-dimensional Li+ diffusion pathways. However, the intrinsic complexity and compositional diversity of high-entropy systems have limited a comprehensive understanding of the correlation between crystal structure, elemental composition, and rate performance, thereby impeding further optimization and practical application. In this study, a high-entropy spinel oxide (Fe0.2Co0.2Ni0.2Cr0.2Zn0.2)3O4 (FCNCZO) is synthesized to investigate its electrochemical properties. The material delivers a high reversible capacity of 551 mAh g–1 at 500 mA g–1 after 110 cycles and maintains an excellent rate capability of 330 mAh g–1 at a high current density of 2000 mA g–1. Density functional theory calculations indicate that the synergistic interaction among multiple metal elements reduces the bandgap and broadens the d-band width. Moreover, the high-entropy effect promotes metal-oxygen orbital hybridization, facilitates charge redistribution, and significantly enhances rate capability. These findings provide new microscopic insights into the high-entropy effect and demonstrate its potential in designing next-generation high-entropy anode materials with superior rate performance for high-power lithium-ion batteries.
The increasing demand for high-capacity energy storage, spurred by the growth of renewable energy, has accelerated the pursuit of cost-effective and sustainable aqueous zinc-ion batteries as a viable alternative to traditional lithium-ion batteries. In this study, a cation-anion coordination cathode material (Zn-MnO2FX) is proposed, which regulates the central valence state of Mn ions by covalently anchoring manganese oxides with Zn ions and F ions to inhibit Jahn-Teller distortion and manganese dissolution. Density Functional Theory calculations elucidate the intercalation of Zn2+ extends the MnO2 layer spacing, reduces ion diffusion barriers, and accelerates ion diffusion, while F– ions repair defects and enhance the electronic conductivity of MnO2, which stabilizes the cathodes and prolongs the life span of batteries. The co-insertion of Zn2+/H+ in MnO2 and the auxiliary effect of Zn4SO4·(OH)6·xH2O on dissolution/deposition were elucidated by analyzing the changes in structure, morphology, and impedance during the cycling process. The Zn-MnO2Fx cathode exhibits a high reversible capacity of 365.5 mA h g–1 at 0.1 A g–1, with remarkable capacity retention of 96.7% after 1000 cycles at 1 A g–1. The initial specific capacity of the flexible yarn battery reaches 112.5 mA h g–1 at 0.1 A g–1. This work adeptly addresses the kinetic-stability balance in cathode materials, offering a pioneering strategy for sustainable and efficient large-scale energy storage.
Understanding and managing charge carrier recombination dynamics is crucial for optimizing the performance of metal halide perovskite optoelectronic devices. In this work, we introduce a machine learning-assisted intensity-modulated two-photon photoluminescence microscopy approach for quantitatively mapping recombination processes in MAPbBr3 perovskite microcrystalline films at micrometer-scale resolution. To enhance model accuracy, a balanced classification sampling strategy was applied during the machine learning optimization stage. The trained regression chain model accurately predicts key physical parameters—exciton generation rate (G), initial trap concentration (NTR), and trap energy barrier (Ea)—across a 576-pixel spatial mapping. These parameters were then used to solve a system of coupled ordinary differential equations, yielding spatially resolved simulations of carrier populations and recombination behaviors at steady-state photoexcitation. The resulting maps reveal pronounced local variations in exciton, electron, hole, and trap populations, as well as photoluminescence and nonradiative losses. Correlation analysis identifies three distinct recombination regimes: 1) a trap-filling regime predominated by nonradiative recombination, 2) a crossover regime, and 3) a band-filling regime with significantly enhanced radiative efficiency. A critical trap density threshold (~1017 cm-3) marks the transition between these regimes. This work demonstrates machine learning-assisted intensity-modulated two-photon photoluminescence microscopy as a powerful framework for diagnosing carrier dynamics and guiding defect passivation strategies in perovskite materials.
Next-generation artificial tactile systems demand seamless integration with neuromorphic architectures to support on-edge computation and high-fidelity sensory signal processing. Despite significant advancements, current research remains predominantly focused on optimizing individual sensor elements, and systems utilizing single neuromorphic components encounter inherent limitations in enhancing overall functionality. Here, we present a vertically integrated in-sensor processing platform, which combines a three-dimensional antiferroelectric field-effect transistor (AFEFET) device with an aluminum nitride (AlN) piezoelectric sensor. This innovative architecture leverages a Zr-rich, leaky antiferroelectric HZO film—a novel material for physical reservoir computing (PRC) devices capable of responding to external stimuli within the microsecond-to-millisecond range. We further demonstrate the 3D AFEFET's adaptability by tuning its discharge current via structural modifications, enabling sophisticated multilayered processing. As an integrated in-sensor processing unit, the 3D AFEFET and AlN sensor array surpass a comparable 2D configuration in both pattern recognition and information density. Our findings showcase a pioneering prototype for future artificial tactile systems, demonstrating the transformative potential of 3D AFEFET PRC devices for advanced neuromorphic applications.
Recent advancements in lead halide perovskites opened up an avenue for vast optoelectronic applications. However, lead toxicity and the complicated synthesis process posed major obstacles to their further practical applications. To address these issues, a facile and robust mechanochemical synthesis of cesium manganese halide (Cs3MnX5, X = halide element) was developed via a highly efficient solvent-free ball milling strategy. This green approach exempted the utilization of any harmful organic solvents, thereby enabling the fast and cost-effective production of lead-free Cs3MnX5 with excellent optical properties. Cs3MnX5 perovskites with mixed halide compositions could also be readily fabricated through this eco-friendly approach at room temperature without any post-purification. Furthermore, the robustness of the ball milling strategy was proved by fabricating zinc-doped Cs3MnX5 perovskites with enhanced thermal stability and ambient stability. These features demonstrated that ball milling was highly efficacious for producing high-quality non-toxic halide perovskites, which could be used in light-emitting diodes.
High-entropy ceramics have exhibited promising application prospects in aerospace, electronic devices, and extreme environment protection. Current powder sintering routes for preparing high-entropy ceramics are hindered by stringent powder requirements, reliance on long-term high-temperature and high-pressure synthesis, as well as compositional inhomogeneity and coarse grains. In this work, the low-temperature glass crystallization method was innovatively introduced into the preparation of high-entropy ceramics. Using garnet-structured rare-earth aluminates (RE3Al5O12, RE is rare-earth elements) as a model system, a series of single-phase RE3Al5O12 ceramics with entropy gradients were successfully synthesized through the glass crystallization method at a low temperature (1000 °C). Notably, the as-prepared (Eu0.2Gd0.2Y0.2Yb0.2Lu0.2)3Al5O12 (HEC) samples exhibited a low thermal conductivity of 3.58 W m–1 K–1 (at 300 K) and a high thermal expansion coefficient (TEC) of 10.85 × 10–6 K–1, representing a 21% reduction in thermal conductivity and a 32% increase in TEC compared to reported Yb3Al5O12 ceramics. The HEC samples also exhibited superior mechanical properties compared to most existing high-entropy ceramics, with a hardness of 22.08 GPa and a Young's modulus of 311.6 GPa. The exceptional comprehensive properties of the HEC samples make them a promising candidate material for thermal barrier coatings (TBCs) and high-temperature structural applications. This investigation confirms that high-entropy ceramics with outstanding properties can be successfully prepared using a glass crystallization method, providing a novel strategy for the low-temperature and pressureless controllable synthesis of single-phase high-entropy ceramics.
The emerging n-type Mg3(Sb, Bi)2-based materials have attracted considerable attention for their excellent thermoelectric performance. Whereas, practical thermoelectric device applications require materials that exhibit not only superior thermoelectric performance but also robust mechanical properties. This work systematically investigates the mechanical and thermoelectric properties of Mg3.2-xCexSbBi0.97Te0.03. The x = 0.04 sample exhibits a Vickers hardness of up to 1012 MPa. The compressive and bending stress–strain curves show that minor doping can enhance the strength while maintaining high plasticity. The superior mechanical characteristics are attributed to dense dislocations and lattice distortions induced by Ce doping. Furthermore, the thermoelectric evaluation shows that the trivalent rare earth Ce element acts as a moderately efficient dopant, leading to increased carrier concentration to 4.55 × 1019 cm–3. However, both the electrical conductivity (σ) and Seebeck coefficient (S) gradually decrease with the increase of Ce doping, particularly at high doping levels (x = 0.04 and 0.06), leading to the slight decrease in power factor. Meanwhile, Ce doping introduces point defects, lattice distortions, and dislocations, thereby enhancing the phonon scattering and reducing the lattice thermal conductivity (кL). As a result, an ultralow кL of ~0.51 W m–1 K–1 and a peak zT of ~1.52 are achieved for the sample of x = 0.02. This work provides some insights into the synergistic enhancement of thermoelectric and mechanical properties in Mg3(Sb, Bi)2-based compounds, inspiring further exploration of their practical applications in thermoelectric devices.
Photoswitchable catalysis provides a non-invasive strategy for dynamically controlling light-driven chemical energy conversion processes. The defining advantage of photoswitchable catalytic systems lies in their unique dual capacity: i) spatiotemporal precision in resolving reactive species generation through optical addressing; and ii) adaptive multifunctionality enabling on-demand switching between distinct active phases, thereby suppressing competing pathways and eliminating undesired side reactions. Current research paradigms remain predominantly anchored in molecular systems, whereas solid-state semiconductor architectures—with their inherent advantages in recyclability and thermal stability—suffer from critical deficiencies in excitation-selective reactivity modulation and interfacial charge transfer kinetics. Here we comment on a recent work, writing in National Science Review, reported spin–orbit coupling-mediated control over anti-Kasha photophysical pathways in semiconductors of carbonylated carbon nitride, enabling optically switchable catalytic dynamics. We further analyzed the profound implications of this work and presented a forward-looking outlook on the future development of the photoswitchable catalysis.
Promising aqueous zinc metal batteries (AZMBs) continue to face significant challenges regarding zinc anode reversibility due to detrimental reactions including hydrogen evolution and corrosion. Herein, the d-band center is used as an “intuitive descriptor” to compare the hydrogen evolution activity of zinc-based transition bimetallic oxides (ZTBOs) of fourth-period transition metal elements, and the advantages of ZnTi3O7 (ZTO) functional protective layer in inhibiting hydrogen evolution and extending the lifespan of the zinc anode are selectively identified. The ZTO exhibits a lower d-band energy level, which affects the adsorption of active H* and exhibits lower hydrogen evolution reaction activity. At the same time, the dense ZTO protective layer provides suitable ion channels to promote the uniform distribution of zinc flux and achieve uniform Zn deposition. Thus, cells with Zn@ZTO anodes exhibit over 6000 h of cycling stability (1 mA cm–2) and a high coulombic efficiency of 99.9% within 1200 cycles. Moreover, when paired with a V6O13 cathode, the assembled full cell exhibits excellent lifespan, retaining 86.9% of its capacity after 5000 cycles at 10 A g–1. This work provides new strategies and insights for designing inorganic protective layers, addressing HER-related challenges, and advancing the practicality of AZMBs.
Beyond traditional rooftop and building-integrated photovoltaics (BIPV), photovoltaic (PV) devices find applications in agrivoltaics, space, and indoor settings. However, the underwater (UW) environment remains largely unexplored. Below 50 m, the solar spectrum shifts dramatically, with only blue-green light (400–600 nm) available. Perovskite solar cells (PSCs), known for their high-power conversion efficiencies (PCEs) and tunable bandgaps, offer potential for this environment. Initially, simulations compared the intensity of the solar radiation based on three models, each based on a different water body, down to a depth of 10 m. The trend of maximum theoretical performance, ranging from 1.5 to 3 eV band gap, was analyzed with respect to depth. In this pioneering study, a wide bandgap PSC, based on FaPbBr3, has been selected to operate underwater. Results were achieved through a complete in-house process encompassing fabrication, encapsulation, and underwater measurement. A 10-day saltwater submersion test of a damaged device confirmed minimal lead release, meeting stringent legal standards for lead in potable water. PV performance was evaluated UW, demonstrating an enhanced conversion efficiency within the first centimeters of water. This enhancement is due to water's optical and cooling properties. This work opens new frontiers for exploration, both for perovskites, traditionally considered unsuitable for humid environments, and for the increasingly human-occupied underwater realm, which is seeing the development of activities such as wine aging and plant cultivation.
This review presents a comprehensive overview of recent advances in supercapacitor electrode materials, with a particular emphasis on the synergistic interactions between electrode materials and electrolytes. Beyond the conventional categorization of materials such as carbon-based materials, conducting polymers, and metal oxides, we focus on emerging nanostructured systems including MXenes, transition metal dichalcogenides (TMDs), black phosphorus, and quantum dots. We highlight how engineering the electrode–electrolyte interface—through the use of ionic liquids, gel-based, and solid-state electrolytes—can enhance device performance by expanding voltage windows, improving cycling stability, and suppressing self-discharge. In addition, we discuss recent insights from density functional theory (DFT) and density of states (DOS) analyses that elucidate charge storage mechanisms at the atomic level. By integrating materials selection, interface engineering, and application-oriented design considerations, this review provides a forward-looking perspective on the development of next-generation supercapacitors for use in flexible electronics, electric vehicles, and sustainable energy systems.
Covalent organic frameworks have emerged as a hot spot in the field of photocatalysis due to their excellent structural tunability, high specific surface area, high porosity, and good chemical stability. Specifically, they exhibit distinctive optoelectronic features by integrating different molecular building blocks with appropriate links, constructing an π-conjugated system, or introducing electron donor–acceptor units into the conjugated framework. The reasonably adjusted band structure yields excellent photocatalytic activity of covalent organic framework materials. In this review, we comprehensively focus on applications of covalent organic framework materials as effective photocatalysts within the realm of hydrogen production, CO2 reduction, pollutant degradation, organic conversion and other aspects. The discussion encompasses synthesis methods and reaction types of covalent organic frameworks. This review also discusses the state-of-the-art research progress, performance optimization strategies and the diverse manifestations of covalent organic framework materials used in photocatalysis. Finally, the main challenges and prospects aimed at further improving the photocatalytic performance of covalent organic frameworks are briefly proposed. By giving us a thorough understanding of the structural complexities of covalent organic frameworks and their essential role in photocatalytic processes, this effort advances our understanding and serves as a guide for the future design and development of novel covalent organic frameworks.
Chronic wounds resulting from diabetes are among the most common complications in diabetic patients. Attributable to poor local blood circulation and an increased risk of infection, these wounds heal slowly and are difficult to treat, posing a significant global health challenge. Herein, we achieved the green valorization of waste liquid from the natural clay-derived zeolite synthesis process and utilized it to fabricate metal-loaded aluminosilicate dressings with pronounced wrinkled structures (wrinkled Cu–AS, Ga–AS, and Ce–AS) through simple procedures. Wrinkled Cu–AS and Ce–AS exhibited strong antibacterial activity against Escherichia coli, Staphylococcus aureus, and Candida albicans, with wrinkled Ce–AS demonstrating notable antibiotic-like effects against C. albicans. Moreover, wrinkled Ce–AS enhanced hemostatic capability, promoted blood cell aggregation and activation, downregulated inflammatory markers (IL-6/TNFα), stimulated angiogenesis (VEGF), and shifted macrophage polarization toward the M2 phenotype, thereby facilitating rapid wound healing. Sprague–Dawley rats tolerated intraperitoneal administration well, with no observable toxicity as well as satisfactory hemolysis and cell compatibility. Notably, in the context of growing demand for natural clay utilization and zeolite production, this work presents a unique green approach for the efficient reuse of zeolite synthesis waste liquid, offering both environmental sustainability and commercial viability. This expands the repertoire of biomedical materials available for treating chronic diabetic wounds.
Silica (SiO2) anodes are promising candidates for enhancing the energy density of next-generation Li-ion batteries, offering a compelling combination of high storage capacity, stable cycling performance, low cost, and sustainability. This performance stems from SiO2 unique lithiation mechanism, which involves its conversion to electroactive silicon (Si) and electrochemically inactive species. However, widespread adoption of SiO2 anodes is hindered by their slow initial lithiation. To address this, research has focused on developing electrochemical “activation protocols” that involve prolonged low-potential holding steps to promote SiO2 conversion. Despite these efforts, the complex and multi-pathway nature of SiO2 lithiation process remains poorly understood, impeding the rational design of effective activation strategies. By introducing a multi-probe characterization approach, this study reveals that, contrary to the previously proposed reaction mechanism of SiO2 anodes, the lithiation process initiates at low potentials with the direct formation of Li4SiO4 and LixSi. Electrochemical activation potential was found to significantly influence the degree of conversion, with 10 mV identified as the optimal cut-off potential for maximizing SiO2 utilization. These findings provide key enablers to unlock the full potential of SiO2 anodes for battery technology.
The exceptional resistive switching characteristics and neuromorphic computational potential of memristors are crucial for advancing information processing in both traditional and non-traditional computing paradigms. However, the non-ideal resistive switching behavior of conventional oxide-based memristors hardly meets the performance requirements for neuromorphic computing applications. Besides, the two-terminal memristors are restricted by their configuration limitations toward multi-field/multi-functional modulation. Herein, this article presents a 2D GaSe/MoS2 heterojunction thin-film transistor with four-terminal (4-T) tuning capability and flexible programming/erasing operations for non-volatile storage. The heterojunction transistor demonstrates an exceptional resistance switching ratio exceeding 107, an ultra-wide modulation range of 10–106, highly reliable stability, and cyclic durability. The in situ Kelvin probe force microscope and dynamic characterization reveal the conduction mediated by defect-induced space charge limitations, as well as the tuning filling process of trap states within the channel by dual-gate terminals. This device functions as a 4-T artificial synapse, capable of achieving basic optoelectronic synaptic operations. The self-denoising and pattern recognition capabilities exhibited by artificial neural networks based on this device serve as excellent examples for developing efficient and energy-saving neuromorphic computing architectures.
Screen printing using metal particle pastes, the current photovoltaic industry metallization standard, provides fast and reliable metal grids for silicon solar cells. Recently, metal complex or reactive metal inks are attracting research interest due to their significantly low cost and higher performance compared to traditional nanoparticle silver pastes. In this work, we demonstrate, for the first time, screen-printed high-efficiency silicon heterojunction solar cells metallized by silver metal complex inks on industrial G1-size (158.75 × 158.75 mm2) wafers. We demonstrate screen-printed Ag metal complex ink grid patterns with continuous fingers ~100–120 μm wide. The printed Ag grid is very thin (~1 μm), which is an order of magnitude thinner than the current ~20–30 μm fingers printed with low-temperature nanoparticle-based pastes. Double printing allows silicon heterojunction devices with efficiencies >20%. This is the highest efficiency so far, to our knowledge, of industrial solar cell precursors using this metallization technology. Simulation results suggested that increasing the thickness of the metal film does not significantly improve efficiency due to the dense, highly conductive films. So, a single print of ~1 μm finger would be enough to produce cells that perform similarly to a ~20 μm thick nanoparticle paste printed cells. Additionally, solar cells printed on G1 wafers with silver metal complex ink required more than 10 times less silver (~0.03 g) compared to those using silver/copper nanoparticle paste (~0.4 g of Ag). These results indicate that metal complex inks are a very promising replacement for silver nanoparticle pastes for industrial-scale metallization in an age of resource scarcity and high costs of noble metals.
As the transition to renewable energy accelerates, sodium metal batteries have emerged as a viable and economical substitute for lithium-ion technology. The unstable solid electrolyte interphase on sodium metal anodes continues to provide a significant challenge to attaining long-term cycle stability and safety. Natural solid electrolyte interphase layers frequently demonstrate inadequate mechanical integrity and deficient ionic conductivity, resulting in dendritic formation, diminished Coulombic efficiency, and capacity degradation. Creating artificial solid electrolyte interphases has emerged as an essential remedy to address these restrictions. This review offers an extensive analysis of artificial solid electrolyte interphases techniques for sodium metal batteries, emphasizing their creation mechanisms, material selection, and structural design. The research highlights the significance of fluoride-based materials, multi-layered solid electrolyte interphase structures, and polymer composites in mitigating dendrite development and improving interfacial stability. Advanced characterization techniques, including microscopy and spectroscopy, are emphasized for examining the microstructure and ion transport properties of artificial solid electrolyte interphases layers. Additionally, density functional theory simulations are examined to forecast ideal material compositions and ion migration paths. This study seeks to inform future developments in artificial solid electrolyte interphases engineering to facilitate enhanced performance, safety, and market viability of sodium metal batteries. Artificial solid electrolyte interphases facilitate next-generation sustainable energy storage systems through new interface designs and integrated analysis.
The LiNixCoyMn1-x-yO2 (NCM) cathode materials have emerged as critical components in lithium-ion batteries due to their high energy and power densities. The co-precipitation method is widely used in laboratory and industry settings to optimize the crystallinity, grain morphology, particle size, and sphericity of precursor materials, directly affecting NCM battery performance. This review addresses the nucleation mechanism and the thermodynamic and kinetic reaction processes of co-precipitation. The comprehensive effects of key parameters on precursor physicochemical properties are also systematically interpreted. Notably, precursor characterization and physicochemical properties, including impurity levels and tolerance limits relevant to production, are highlighted. Finally, optimization strategies for developing high-quality precursor materials toward commercialization are proposed. This systematic review provides a deeper understanding of precursor optimization and advances relevant theories for the development of NCM cathode materials.
Sluggish electrode kinetics and polysulfide dissolution severely hinder room-temperature sodium-sulfur batteries (RT Na-S) from achieving high-theoretical capacity and low cost. Metal-based catalysts are often used to absorb polysulfide intermediates against the shuttle effect in Na-S batteries, but rationalization of an electrode pore structure to improve battery performance is ignored. Herein, a rational micropore/mesopore network structure of macadamia nut shell-derived carbon is constructed as a carbon/sulfur cathode by tuning the ratio of micro to mesopore. The cathode simultaneously boosts mass transport for high-rate performance while confining the shuttle effect for long cycles, thus delivering excellent Na-storage performance with high capacities of 912 mAh g–1 at 0.1 A g–1 and 360 mAh g–1 at 5 A g–1, ranking the best among all reported plain carbon-based sodium-sulfur electrodes. This work holds great promise for biomass-derived inexpensive plain carbon-based electrodes in practical high-rate applications, while shedding light on the fundamentals of pore structure effects of a carbon electrode on high-performance batteries, thus possessing universal significance in the designs of rational pore structures in energy conversions.
As a forefront energy storage technology, lithium-ion batteries (LIBs) have garnered immense attention across diverse applications, including electric vehicles, consumer electronics, and medical devices, owing to their exceptional energy density, minimal self-discharge rate, high open circuit voltage, and extended lifespan. However, despite their remarkable advancements and widespread commercialization, LIBs continue to face critical challenges, particularly the demand for even higher energy density, which inhibits their performance in high-power applications such as electric and hybrid electric vehicles. This review presents a comprehensive analysis of the fundamental limitations hindering LIBs from achieving superior energy density and long-term electrochemical stability. The discussion is systematically structured around four key components: cathode materials, anode materials, separators, and current collectors, with a particular emphasis on the challenges, emerging strategies, and future perspectives. By delving into recent breakthroughs in novel material architecture, electrode design optimizations, and the selection of advanced separators and current collectors, this work provides an in-depth examination of innovative approaches aimed at enhancing battery performance. Furthermore, this review explores pivotal factors such as interfacial stability, ion transport kinetics, and degradation mechanisms that significantly impact the longevity, safety, and efficiency of LIBs. By critically evaluating these aspects, it offers valuable insights into the trajectory of LIB development, helping to shape the next generation of high-performance energy storage solutions.