A novel carbon material with edge-dominant pyridinic nitrogen doping is synthesized from tannic acid (TA), an agricultural byproduct, using a quick and straightforward two-step microwave irradiation technique. Tris(2-aminoethyl)amine (TAEA) plays a dual role in this process, acting as a condensing agent for TA in the initial step and providing nitrogen for the pyridinic structure in the second step. This approach results in a distinctive carbon structure (C–TA/TAEA) characterized by enhanced graphitic features, fewer imperfections, and similar hydrophilicity. The edge pyridinic configuration lowers the desorption energy of V3+ complexes and the deprotonation energy of VO2+ complexes, thereby boosting the catalytic activity for vanadium ion redox reactions (VIRR) by influencing the rate-limiting steps of both positive and negative side VIRRs. When applied to commercial thermal-treated graphite felt (T-GF/[C-TA/TAEA]), the material demonstrates stable performance during vanadium redox flow battery (VRFB) single cell testing, even at 500 mA cm−2, showing improved energy efficiency (EE) and discharge capacity compared to T-GF. Furthermore, when applied to pristine graphite felt (GF/[C–TA/TAEA]), the material maintains a 94.12% discharge capacity retention rate over 1000 cycles at 400 mA cm−2, underscoring its potential as an eco-friendly, energy-efficient treatment method for producing VRFB electrodes.
As demand for lithium-ion batteries increases, the supply of materials is increasingly constrained by their geographical concentration. This has spurred significant research into recycling spent batteries to enhance resource circulation. Currently, commercially applied recycling methods (such as pyrometallurgy and hydrometallurgy) face environmental and economic challenges, including waste acid and gas generation, high-temperature heat treatment, and operational complexity. A promising alternative is the carbothermic reduction process, which operates at lower temperatures, minimizing costs and environmental emissions. However, this method still requires large quantities of external reducing agents. Therefore, this study aims to introduce a simplified direct carbothermic reduction (SDCR) process. The SDCR process leveraged carbon conductive materials and organic binders within the electrode as reducing agents. Additionally, the high compaction state created a conducive environment for reducing gases, promoting efficient reduction and material recovery. This approach reduces the reliance on external reducing agents and streamlines the re-upcycling process, making it commercially viable.
In this study, gallium vanadium oxide mixed-oxide material was synthesized using a simple solid-state reaction followed by an annealing process. Flexible, free-standing gallium vanadium oxide-based composite electrodes were fabricated and evaluated in various energy storage systems, including lithium-ion batteries, sodium-ion batteries, lithium-ion capacitors, and sodium-ion capacitors. Experimental results demonstrated the remarkable versatility of gallium vanadium oxide. The free-standing electrode based on gallium vanadium oxide mixed-oxide materials achieved impressive discharge capacities of 571 mAh g−1 for lithium-ion batteries and 202 mAh g−1 for sodium-ion batteries at a 1 C-rate. These values are close to the theoretical capacities of 588 mAh g−1 for lithium-ion batteries and 236 mAh g−1 for sodium-ion batteries, indicating the high efficiency and performance of the gallium vanadium oxide free-standing electrode. The hybrid-ion capacitors further showcased gallium vanadium oxide's capabilities, with lithium-ion capacitors delivering energy and power densities of 178.24 Wh kg−1 and 16.6 kW kg−1, respectively, and sodium-ion capacitors achieving 130.74 Wh kg−1 and 13.30 kW kg−1. Density functional theory calculations revealed that the incorporation of gallium lowers the formation energy of stable defects in V2O5 during ion intercalation and enhances electrical conductivity by reducing the bandgap. The combined experimental and theoretical analysis positions gallium vanadium oxide as a versatile and highly promising material for next-generation sustainable energy storage devices.
LiCoO2 is promising for aqueous lithium-ion batteries due to its simple production processes and high energy density. However, LiCoO2 exhibits poor cycle life in aqueous electrolytes, primarily attributed to H+ intercalation, interfacial reactions, and irreversible phase transformation, which substantially impedes its practical application. Herein, an integrated surface-to-bulk Nb modification strategy combining LiNbO3 surface coating and gradient Nb doping (N-LCO@LNO) is proposed to enhance the cycling stability of LiCoO2. The LiNbO3 surface coating serves as a physical barrier to suppress side reactions, while the gradient Nb doping stabilizes the bulk structure and inhibits spinel phase transition. Density functional theory calculations further reveal that this synergistic modification strategy can significantly suppress the structural degradation induced by electrophilic attack of H+. As a result, the N-LCO@LNO electrode delivers a high-rate capability of 117.1 mAh g−1 at 4 C and a long-life stability with 71.4% capacity retention after 100 cycles at 0.5 C, far outperforming the unmodified LiCoO2 electrode with only 11.1% capacity retention. This study presents a highly promising modification strategy that facilitates the effective utilization of LiCoO2 in aqueous electrolytes.
Poor wettability of poly(triarylamine) (PTAA) surfaces and insufficient control over residual PbI2 clusters remain critical bottlenecks limiting the performance of PTAA-based p-i-n perovskite solar cells (PSCs). Herein, we introduce an effective interface engineering strategy through the incorporation of the ionic liquid 1-butyl-3-methylimidazolium acetate (BMIMAc). Owing to its strong affinity for the perovskite precursor solvent (N,N-dimethylformamide, DMF), BMIMAc significantly enhances PTAA wettability, promoting the formation of uniform and defect-passivated perovskite films. In addition, BMIMAc modulates the energy level alignment of PTAA, facilitating more efficient hole extraction and transport across the interface. More importantly, BMIMAc interacts with PbI2 to decelerate perovskite crystallization kinetics, enabling a more complete conversion of PbI2 into the perovskite phase. This synergistic regulation yields perovskite films with enlarged grain sizes, reduced trap densities, and suppressed nonradiative recombination losses. Benefiting from these advances, the optimized PTAA-based p-i-n PSCs achieve a record-high power conversion efficiency of 25.10% with significantly enhanced operational stability.
Renewable energy is critical to building a sustainable society, but its true potential can only be unlocked by developing efficient, environmentally friendly energy storage systems. Advances in storage technologies, including cost-effective and green materials, are quickly becoming the cornerstone of sustainable energy solutions. The most effective battery technology available now is lithium-ion batteries (LIBs). However, the sustainability of battery material production and the degradation of LIB functionality at subzero temperatures pose significant challenges, highlighting the urgent need for alternative and sustainable low-temperature (LT) electrode materials. To overcome these issues, a green synthesis approach is proposed to fabricate SnO2 nanoparticles using an aqueous extract of banana peel, while the leftover peel serves as a carbon precursor to produce a SnO2/hard carbon composite. The optimized SnO2/hard carbon (7:3) composite was used as the anode and showcased a remarkable reversible capacity of 1110 mAh g−1 at room temperature and retained about 660 mAh g−1 at −20 °C and 100 mA g−1 after 100 cycles, with a capacity of 383 mAh g−1 even at −30 °C. Stable cycling performance was achieved by the synergistic interaction of SnO2 and hard carbon, which improved lithium-ion diffusion and mitigated volume expansion. This eco-friendly and scalable approach shows great promise for developing high-performance anodes for the next generation of LT LIBs.
The structural modulation of the inner Helmholtz layer is crucial to enhance the cycling stability of Zn anode interface. A water-rich inner Helmholtz layer normally induces uncontrollable zinc dendrites, hydrogen evolution and corrosion, severely compromising the cycle life of the zinc anode. Therefore, in this work, green and non-toxic dipropylene glycol dimethyl ether (DMM) is used as an additive to remodel the inner Helmholtz layer. Both experimental and computational results show that DMM is zincophilic and can preferential adsorb on the zinc surface for the occupation of the inner Helmholtz layer. Meanwhile, DMM contains two hydrophobic methyl groups, which can repel water molecules remaining after solvent removal, and build a lean-water inner Helmholtz layer to avoid continuous contact between water molecules and zinc anode. The quartz crystal microbalance with dissipation test intuitively and accurately reflected the adsorption behavior of DMM on the surface of zinc anode, and realized the leap from qualitative analysis to quantitative analysis. The Zn//Zn symmetric cells with DMM electrolytes have a stable cycle life of over 1100 cycles at 2 mA cm−2 and 0.5 mAh cm−2. In addition, Zn//PANI cell with DMM electrolyte can maintain 90% capacity retention over 1000 cycles at 1 A g−1.
Lattice oxygen participation is crucial for oxygen-evolution reaction (OER) performance, but stabilizing the active high-valence cation remains a major challenge. This study focuses on iron oxyhydroxide (FeOOH), which exhibits a delicate balance between high-valence states and stability. A heterostructure (CeO2/FeOOH) with an electron-rich, high-valence-state interface was synthesized via a simple co-precipitation method. Due to the work-function disparity between CeO2 and FeOOH, electron accumulation occurs in CeO2, while FeOOH attains a high-valence state. This enhanced valence state strengthens Fe–O covalency, facilitating lattice oxygen participation in oxygen-evolution reaction. Furthermore, electron-abundant CeO2 functions as a redox buffer, where the electron-reservable Ce3+/Ce4+ redox couple stores excessive oxygen and donates electrons to stabilize high-valence FeOOH. By incorporating this “redox-buffering system,” Fe dissolution was minimized, significantly improving catalyst stability under harsh oxidizing conditions. The anion exchange membrane electrolyzer exhibited outstanding performance, delivering a current density of 500 mA cm−2 at 1.69 V, with remarkable stability over 100 h at 1 A cm−2. These findings provide a new strategy for stabilizing high-valence-state oxygen-evolution reaction catalysts, offering valuable insights for designing efficient and durable electrochemical systems.
The development of efficient, cost-effective, and durable electrocatalysts for the hydrogen evolution reaction (HER) is critical for advancing sustainable energy systems and enabling the widespread adoption of hydrogen-based energy technologies. In this study, we discover a stable hexagonal V2B2 monolayer that serves as a promising HER catalyst via an unbiased swarm-intelligence structural method as implemented in CALYPSO code. First-principles calculations show that the predicted V2B2 monolayer exhibits excellent metallic properties and promising catalytic activity for HER, suggesting CALYPSO's utility for accelerating the discovery of efficient electrocatalysts. Further doping engineering, incorporating transition metals (TM′ = Sc, Y, Ti, Zr, Hf), reveals that the introduction of Sc, Y, and Zr significantly enhances the catalytic performance. Bader charge analysis reveals a linear correlation between the electron gain by the hydrogen atom and ΔGH*, suggesting that this relationship could serve as an effective descriptor for HER activity in TM'-doped V2B2 systems. Our findings provide valuable insights into nonprecious HER electrocatalysts and contribute to a deeper understanding of high catalytic performance in newly proposed 2D HER catalysts.
Future wearable electronics require sustainable power sources, and nanogenerators offer promising solutions to convert ambient mechanical energy to electricity while ensuring flexibility, durability, and practical deployment. This work demonstrates a textile-based piezoelectric nanogenerator (T-PENG), which is a durable and scalable energy-harvesting system, using the inherent strength of 2D materials to elevate the performance metrics significantly. Screen printable 2D graphene ink was used for developing the textile-based flexible electrodes. The composite layer was prepared using zinc oxide (ZnO) enclosed molybdenum disulfide (MoS2) (MoS2@ZnO) and a screen printable paste. The incorporation of 2D MoS2 into the T-PENG system significantly enhances its output performance. This improvement is further validated by COMSOL computer simulations, which align closely with the experimental findings. At 10 wt% of MoS2, d33 value of our device reaches ~5.67 pC N−1, an approximately threefold improvement over the MoS2-free device. Furthermore, T-PENG resulted in a significantly high open-circuit voltage (Voc) of ~60 V, and a peak power density (J) of 126.84 mW m−2. Moreover, T-PENG demonstrates high durability and flexibility while retaining ~92% of its output power over 3 months and sustaining ~90% efficiency after 500 bending cycles. T-PENG demonstrated the ability to power over 60 blue light emitting diodes (LEDs) and functions as a self-powered sensor. These advancements position MoS2 as a significant material for next-generation multifunctional smart textiles.
To boost the practical energy density of lithium-sulfur batteries, replacing conventional solvating electrolytes with sparingly solvating ones has shown promise by enabling solid-state sulfur conversion and reducing electrolyte consumption. However, this approach often compromises sulfur redox kinetics. This study reports a new sulfur conversion pathway distinct from both traditional solvated and sparingly solvated mechanisms. Specifically, sulfur is converted into a mixture of solid and solvated lithium polysulfides (LPSs). Such a hybrid solid/solvating conversion pathway is achieved using a newly formulated moderately solvating electrolyte, accomplishing both lean-electrolyte operation and fast conversion kinetics for lithium-sulfur batteries. Methoxyacetonitrile (MAN) is selected as the solvent to formulate the moderately solvating electrolyte due to its high relative permittivity (21) that contributes to a high Li+ conductivity (11.7 mS cm−1 for 1M lithium bis(trifluoromethane sulfonyl)imide in MAN) and low donor number (14.6 kcal mol−1) that reduces the solubility to LPSs to 1/6 of that in mainstream solvating electrolytes. The as-formulated MAN electrolyte enables sulfur cathodes to operate at a low electrolyte-to-sulfur ratio of 2 μL mg−1 and a low cathode porosity of 52%, displaying excellent prospects for boosting both gravimetric and volumetric energy density.
Biomass-derived carbon for CO2 capture is significant for reducing carbon emissions and recovering C1 resources, contributing to zero-carbon goals. However, developing biomass-based porous carbon with high CO2 capture while reducing regeneration energy consumption remains challenging. This study leverages the tunable pore structure and photothermal properties of biomass-based carbon, integrating adsorption and solar-driven desorption for efficient, low-energy CO2 capture. Specifically, mechanical compaction increased the ultramicropore volume of the porous carbon by 25%, leading to a corresponding 25% enhancement in CO2 adsorption capacity. Theoretical calculations and correlation analyses further elucidated that ultramicropore volume, nitrogen doping, and oxygen doping play significant roles in CO2 adsorption. Under one-sun illumination, the surface temperature of the prepared porous carbon rapidly rose to 57.1 °C within 6 min and stabilized around 71.0 °C, resulting in a regeneration efficiency of 75%. These findings provide valuable theoretical and practical insights for the development of high-efficiency, low-energy CO2 capture technologies.
Nanocomposite technology is an effective strategy to enhance the performance of capacitive deionization (CDI). However, the poor interfacial interactions between the nanofillers and matrices limit their further optimization and commercial application. Here, we developed an interface engineering strategy to prepare a high-strength and high-toughness fiber electrode based on holey reduced graphene oxide (HRGO) and carboxylated carbon nanotubes (CCNT) through introducing borate bonds as bridging interactions. The interface interaction between HRGO and CCNT is significantly enhanced by the formation of dynamic cross-linked borate bonds, which not only effectively prevent π-π stacking and construct hierarchical ion transport channels to enhance ion transport efficiency and reaction kinetics, but also significantly improve mechanical stability and long-cycle performance based on self-healing properties in the fiber electrode. This configuration showed remarkably enhanced desalination capacity (30.6 mg g−1) and higher desalination rate (6.12 mg g−1 min−1), with cycling performance exceeding 90%, which exceeds previously reported values. Density functional theory calculations further reveal the mechanism by which the nanocomposite interface affects the CDI performance. Based on this excellent performance, we established a recirculating desalination hydrogen production system consisting of multiple CDI units connected in series with a hydrogen production unit. This effective strategy opens a new way to optimize the nanocomposite interfaces and achieve efficient electrochemical reactions.
The deployment of safe and high-energy density lithium metal polymer batteries (LMPBs) still requires further advances in the quest for new solid polymer electrolytes (SPEs). In this regard, salt anions have a decisive role in the overall SPE performance. While lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was chosen earlier to have a highly flexible sulfonimide center and an extensively delocalized negative charge, it still suffers from several drawbacks ascribed to its poor interfacial compatibility with the lithium metal (LiM) anode and the fact that it is a PFAS. In this work, a novel lithium salt is cunningly designed, aiming to combine the advantages of previously reported lithium bis(fluorosulfonyl)imide (LiFSI) and lithium bis(difluoromethanesulfonyl)imide (LiDFSI) to overcome the limitations of the state-of-the-art SPE based on LiTFSI/poly(ethylene oxide) (PEO). The SPE containing the developed (difluoromethanesulfonyl)(fluorosulfonyl)imide (LiDFFSI) salt presented reduced interfacial resistance and improved compatibility with the lithium metal (LiM) anode compared with LiTFSI/PEO, enabled by the formation of a stable, uniform, and ionically conductive solid–electrolyte interphase (SEI). In addition, LiDFFSI-based SPEs demonstrated a prolonged cycling stability, achieving over 125 cycles at C/10 with minimal capacity fading in LiM||LiFePO4 cell configuration. These findings evidence how a rational design of the lithium salt chemistry allows tuning the formed SEI, directly impacting the overall SPE performance. Thus, LiDFFSI is presented as a promising alternative lithium salt to improve electrochemical performance and interfacial stability in next-generation LiM batteries.
Real-time monitoring of plant nutrient levels, particularly phosphate, is essential for optimizing plant growth and addressing nutrient imbalances in precision agriculture. Conventional sensors mostly suffer from poor stability, reproducibility, matrix effects, and high costs, limiting their scalability and practical application. To overcome these challenges, a deep learning-integrated remote-gate field-effect transistor sensor utilizing a plant-derived graphene electrode is introduced for enhanced performance and reliability. These solution-processed graphene electrodes, composed of cellulose nanocrystals from plant fibers, are functionalized with phosphate-capturing ferritin and serve as the sensing surface, capacitively coupled to a commercial n-type field-effect transistor to address device variability issues. Deep learning integration significantly improved accuracy, enabling robust and precise phosphate detection. The sensor demonstrates a sensitivity of 14.1 mV dec−1 after the pH correction, a coefficient of variation of responses below 5%, and a 1 ng mL−1 (1 ppb) detection limit. As a proof-of-concept, phosphate levels in Hoagland solution, a standard plant nutrient medium, were monitored, achieving an r2 of 0.951 and a coefficient of variation of 5.39%. A handheld prototype system further demonstrates its potential for on-site continuous monitoring. This sustainable and cost-effective approach provides a scalable solution for real-time phosphate detection with high sensitivity and reproducibility, meeting agricultural demands.
The escalating demand for lithium-ion batteries highlights the critical need for alternative lithium sources beyond limited terrestrial reserves. Seawater offers a promising yet challenging lithium resource due to its sub-ppm level Li+ concentration and the presence of competing cations (Na+, K+, Mg2+, and Ca2+). Here, we present a multilayer graphene membrane decorated with α-phase Al2O3 networks (α-Al2O3/MLG) as a selective and durable platform for lithium extraction from seawater. This membrane leverages van der Waals gaps at Al2O3–MLG heterointerfaces and vertical channels formed at MLG grain boundary defects to achieve high Li+ selectivity. By integrating the membrane into an electrodialysis system, a stable Li+ flux of 0.084 mol h m−2 was maintained over 100 h, which resulted in lithium purity and recovery rates of 88.9% and 88.6% from artificial seawater over three extraction cycles. These findings demonstrate the membrane's potential for selective lithium extraction from seawater while minimizing competing ion transport.
The thin zinc anode in zinc-ion batteries offers the advantages of high energy density and low cost. However, issues such as uneven zinc stripping and dendrite growth significantly reduce the cycling life and safety of the battery. To address this, this study proposes a novel zinc anode construction strategy based on a graphite paper substrate, which significantly improves the reversibility of zinc deposition/stripping by regulating the distribution of the interfacial electric field. Compared to traditional copper foil-based substrates (Cu foil@Zn), the zinc deposition layer formed on the graphite paper substrate exhibits a more uniform morphology and superior electrochemical performance. Experimental results show that the Gr paper@Zn anode surface presents a brighter metallic luster, with a mass reduction of approximately 16% compared to the Cu foil@Zn. SEM and XRD analyses confirm that the graphite paper substrate promotes the formation of a uniform and dense Zn (002) crystal face orientation deposition layer, while the Cu foil substrate forms a columnar crystal structure with Zn (101) orientation. Furthermore, the Zn||I2 full battery assembled with Gr paper@Zn retains 75.1% of its initial capacity after 10 000 cycles at a high current rate of 10 C. The Zn||I2 large-area pouch battery maintains 81.2% of its capacity after 800 cycles at a current of 0.8 A. More importantly, the assembled Zn||I2 multilayer pouch battery delivers an Ah-level capacity (1.67 Ah) and maintains 89.9% of its capacity after 100 cycles. This work provides new interface engineering insights for the design of high-performance thin zinc anodes.
Molecular dynamics simulations were conducted at temperatures of 298.15, 273.15, 253.15, and 233.15 K on three organic electrolytes, composed of 1 m NaPF6 dissolved in strongly coordinating diglyme (DG), a mixture of DG and weakly coordinating Tetrahydrofuran (THF) with a 2:8 volume ratio, and a mixture of DG, THF, and weakly coordinating 1,3-dioxolane (DOL) with a 2:4:4 volume ratio, respectively, hereafter denoted as ND, NDT, and NDTD electrolytes for sodium-ion batteries. The studies indicate strong Na+–DG coordination that leads to a vehicular mechanism, in the sense that Na+ persists in migrating together with strongly coordinating DG in the first coordination shell at all the temperature ranges. Such a vehicular mechanism hinders Na+ migration in the ND electrolyte. In contrast, the introduction of weakly coordinating molecules, such as THF in the NDT electrolyte and THF/DOL in the NDTD electrolyte, considerably perturbs Na+ solvation with various coordinating configurations that include Na+–THF and/or Na+–DOL as well as Na+– contact-ion pairs. Such diversity of the coordinating configurations significantly improves Na+ migration, especially in the NDTD electrolyte, which has the highest ionic conductivity as well as the fractional ionic conductivity of Na+ of 3.68 ± 0.36 and 1.32 ± 0.11 mS·cm−1, respectively, even at a low temperature of 233.15 K.
Polyaniline (PANI) exhibits remarkable electrical conductivity and mechanical flexibility, rendering it widely applicable in flexible electronic devices. For instance, it serves as a channel layer material in Organic Electrochemical Transistors (OECTs). In OECTs, the conductivity of the channel layer plays a pivotal role in dictating the switching speed and current-carrying capacity of the device. Proton acid doping represents an efficacious approach to enhancing the conductivity of polymers. However, the efficiency of direct doping of protic acid is low, thereby imposing limitations on the conductivity of polyaniline. In this study, ultrafast photoexcitation was implemented to efficiently improve the conductivity of camphor sulfonic acid (CSA) doped PANI films. Upon reaching a laser fluence of 166.2 mJ cm−2, the conductivity of PANI films experienced a remarkable increment of nearly four orders of magnitude, soaring to 117.6 S m−1, while its sheet resistance decreased to 170.9 Ω sq−1. Meanwhile, fs-laser-treated PANI-CSA films exhibited excellent stability. The PANI-based OECT device was prepared, and the transconductance escalated from 0.113 to 0.503 mS, representing an increase exceeding fourfold. Our work provides a simple, eco-friendly, and sustainable processing technology for the preparation of high-performance PANI flexible conductive films, showing great application potential for flexible electronic devices.
The development of safe lithium metal batteries (LMBs) is critical for practical applications with high-energy density demanding. In this study, a phosphorus-containing diethyl vinylphosphonate (DEVP)-based gel polymer electrolyte (PD-VI GPE) with high ionic conductivity of 6.38 mS cm−1 is prepared by in situ γ-ray radiation polymerization. The PD-VI GPE induces the formation of a uniform, dense fluorine-, and phosphorus-rich solid electrolyte interphase (SEI) in Li||Cu coin cells, effectively suppressing interfacial side reactions and enabling stable lithium deposition. Pouch cells assembled with the PD-VI GPE (2 g Ah−1) exhibit a specific energy of 420 Wh kg−1 with 89% capacity retention over 80 cycles. A novel in situ separator thermal shrinkage assay reveals that the PD-VI GPE-coated Celgard separator maintains structural integrity at 129 °C. Phosphorus-functional groups in the PD-VI GPE act as oxygen radical scavengers, inhibiting cathode-derived O2 evolution in abusive conditions. Thus, LMBs assembled with the PD-VI GPE demonstrate suppressed thermal runaway and mechanical abuse tolerance. This study establishes a material design paradigm that concurrently addresses interfacial stability and safety challenges, paving the way for the application of LMBs in energy systems with high-safety requirements.
The photocatalytic behavior of covalent organic frameworks (COFs) for carbon dioxide (CO2) reduction is dependent on the structure and physicochemical properties; CO2 photoreduction performance is generally influenced by multiple effects rather than a single variable. Rational design and construction of donor (D)-acceptor (A) type COFs have emerged as an ideal strategy for improving photocatalytic CO2 reduction performance. However, it is still challenging to unveil the influence of building blocks on catalytic activity and selectivity of CO2 conversion in D–A COFs. Herein, we report a modified solvothermal method to construct β-ketoenamine-linked COFs based on a one-step Schiff base condensation reaction. By employing 1,3,5-triformylphloroglucinol (TP), which enables both chemical stability and crystallinity of COFs as the electron acceptor, and 1,3,5-tris(4-aminophenyl)triazine (TAPT), 2,4,6-tris(4-aminophenyl)pyridine (TAPP), and 1,3,5-tris(4-aminophenyl)benzene (TAPB) as the electron donors, respectively, we synthesized three distinct COF materials with different intensities of the D–A interaction, based on the molecule design, to regulate the microenvironment for CO2 photoreduction in pure water. The incorporation of D–A moieties into COFs remarkably accelerates charge separation and transport via enhanced D–A interaction or reinforced charge density difference. TP-TAPB COF, featuring the strongest D–A interaction, exhibited the highest CO production rate of 464.6 μmol g−1 with nearly 100% selectivity, 7.2 times higher activity than TP-TAPT.
Aqueous zinc battery promotes great interest due to its high safety and significant energy density. However, the Zn anode shows severity of dendrite growth and hydrogen evolution reaction (HER). Addressing these challenges requires effective manipulation of the inner Helmholtz plane (IHP). Thereby, we secure a novel strategy for generating water-locking IHP through the in-situ growth of a hygroscopic Zn-ethanolamine (Zn-EA) protective layer on the Zn surface. This layer forms via coordination between ZnCl2 salt and ethanolamine, effectively reducing the intermediate/free water. Moreover, ethanolamine contains zincophilic sites (C–O and –NH2) further promote the uniform Zn deposition. The in-situ Raman confirms the ability of the hygroscopic layer to lock the active water away from the Zn surface. Therefore, Zn-EA@Zn anode exhibits an impressive life stability of 288 h at 20 mA cm−2 and 20 mAh cm−2 with an extended lifespan of 2100 h at 1 mA cm−2 and 1 mAh cm−2. Furthermore, the Zn-EA@Zn||Cu demonstrates 100% Coulombic efficiency over 4275 cycles, while Zn-EA@Zn ||V2O3/NC full cell retains a specific capacity of 170 mAh g−1 at 5 A g−1 after 1000 cycles, and the pouch cell maintains 0.5 mAh cm−2 after 460 cycles at 2 mA cm−2. Therefore, this approach is paving the way for the development of advanced zinc metal batteries.
LiNi0.8Co0.1Mn0.1O2 (NCM811), a high-nickel layered oxide, has emerged as a frontrunner for next-generation lithium-ion batteries (LIBs) due to its high energy density, excellent rate performance, and cost-effectiveness. However, NCM811 cathodes face multifaceted challenges, including cation mixing, microcracking, and residual lithium compounds, necessitating a comprehensive understanding for addressing these critical issues. In this review, we provide an in-depth analysis of recent advancements, presenting actionable insights into effective strategies to address the key issues in the NCM811 cathode and proposing pathways for optimizing NCM811 cathodes in LIB applications. Additionally, the forward-looking perspectives are explored in this review, highlighting the role of advanced material characterization techniques, theoretical modeling, and computational simulations in overcoming the inherent limitations of NCM811 cathodes. By synthesizing current knowledge and technological advancements, this review aims to serve as a foundational resource for researchers and industry professionals striving to enhance the performance and accelerate the commercialization of NCM811 cathode materials, contributing to the future of energy storage solutions.
CdS-based photocatalysts offer an efficient route for simultaneous photocatalytic hydrogen evolution and benzyl alcohol oxidation to value-added chemicals. However, the rapid charge recombination, poor oxidation capabilities, and strong photocorrosion of CdS, when used alone, can lead to low productivity of H2 and benzaldehyde. Herein, we present a novel S-scheme heterojunction through coupling CdS with Fluorenone-COF as the promising oxidation end. The suitable band level and active center of the fluorenone moiety impart strong oxidative capabilities to the fluorenone-based COFs, enabling them to efficiently catalyze the oxidation of benzyl alcohol with a low reaction energy barrier. Furthermore, the intrinsic electric field of the S-scheme heterojunction significantly improves the separation and mobility of photoinduced charge carriers, while effectively suppressing charge recombination, which in turn reduces the corrosive effect of photogenerated holes on CdS. Consequently, the heterojunction significantly improved the yield of both benzaldehyde and hydrogen. In the presence of Pt as a cocatalyst, the production rates of H2 and benzaldehyde reached 23.38 and 17.36 mmol g−1 h−1, respectively. This work not only addresses the challenges associated with the utilization of electron holes but also provides an effective green and low-carbon pathway to overcome the challenges of low efficiency and high cost in photocatalytic hydrogen production.
Li metal anodes, with high theoretical capacity (3860 mAh g−1) and low redox potential, are promising for high-capacity rechargeable batteries. Especially, ultra-thin Li metal anodes can improve energy density and minimize lithium excess. However, their poor processability leads to non-uniform Li layers and unstable plating/stripping behavior. In this study, we present a current collector interphase (CCI)-based strategy using a Cu foil coated with a lithiophilic Si3N4 layer, followed by molten Li dip-coating to form around 20 μm Li layer. Furthermore, the scalable dip-coating method, compatibility with large-area current collectors (up to 100 cm2), and stable cycling in pouch cells demonstrate the practical viability of the proposed SNLMA design for commercial lithium metal batteries. During the process, an in-situ Li–Si–N alloy gradient interphase forms at the interface, enhancing wettability and mechanical integrity. This unique gradient CCI provides synergistic lithiophilicity and structural stability, enabling high-performance Li metal batteries. The resulting LixSiy and LixNy phases reduce nucleation barriers and enable uniform Li deposition. As a result, the Si3N4–Li anode paired with a high-loading LCO cathode (22 mg cm−2) achieved 83% capacity retention after 100 cycles. This work offers a scalable and practical CCI design for next-generation Li metal batteries.
Lithium–sulfur batteries (LSBs) suffer from sluggish lithium polysulfides (LiPS) conversion and severe interfacial instability, which limit their rate performance and cycle life. Herein, we report a multifunctional interlayer comprising Mo2C nanoparticles confined within a nitrogen- and phosphorus-codoped amorphous carbon matrix supported on reduced graphene oxide (MNPG). H3PMo12O40 was chosen as a final polyoxometalate (POM) precursor because it was transformed into the tubular nanoparticles, while Na3PMo12O40 was converted to irregular micrometer-sized particles. In particular, the hierarchical structure of MNPG is synthesized via electrostatic self-assembly of POM and pyrrole on graphene oxide, followed by thermal transformation. The embedded Mo2C domains act as efficient redox mediators that accelerate LiPS conversion, while the polar doped carbon shell suppresses parasitic reactions and facilitates ion transport. Consequently, the MNPG-coated separator allows LSBs to deliver a high specific capacity of 1549 mAh g−1 at 0.1 C and 802 mAh g−1 at 5.0 C, along with 81.1% capacity retention after 200 cycles. This study provides a straightforward and effective interfacial engineering strategy that combines redox-mediating domains and transport regulation within a unified structure to overcome key bottlenecks of LSBs.
Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10−4 S cm−1) and anodic stability (>4.4 V vs Li+/Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li+ transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.
Achieving multi-spectral stealth across visible and infrared (VIS-IR) bands is crucial for military and national defense security in diverse environments. However, the coordination of spectrally selective thermal radiation with angle-insensitive color modulation in flexible architectures remains a significant challenge. Herein, we present a chromatic meta-textile enabling flexible VIS-IR multispectral stealth. The stochastic fiber structure with embedded colorants provides wide-gamut coloration, exhibiting negligible color difference between stealth film and different backgrounds as low as 0.4 L*a*b. Simultaneously, the architecture achieves ultralow emissivity (ε = 0.1) in mid-wave infrared (MWIR, 3–5 μm) and long-wave infrared (LWIR, 8–14 μm) bands for infrared stealth, while maintaining high emissivity (ε = 0.58) in the 5–8 μm nonatmospheric window to enable passive radiative cooling. This design features excellent VIS wide-angle compatibility and optical durability, enabling effective stealth in various environments. This integrated multispectral stealth capability, combined with inherent mechanical flexibility and omnidirectional optical stability, positions the structure as a promising solution for next-generation VIS-IR compatible stealth systems.
The hydrazine oxidation-assisted hydrogen generation system significantly expands the applicability of hydrogen production technology. However, the complex intermediate transformations involved in the hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER) desperately need the development of dual-functional catalysts. Manipulating the d-band center of metal catalysts has been identified as one of the most effective approaches to enhance catalytic activity. Herein, Ir nanoparticles (NPs) anchored in B, N-codoped porous carbon (Ir@BNC) were developed and demonstrate excellent performances for both HER and HzOR in an alkaline medium, achieving 10 mA cm−2 at −25 and 18 mV, respectively. The overall hydrazine splitting (OHzS) electrolyzer reaches 200 mA cm−2 with a cell voltage of just 0.68 V. The direct liquid N2H4/H2O2 fuel cell (DHHPFC) assembly with Ir@BNC can achieve a maximum power density of 199.2 mW cm−2 at room temperature. Furthermore, an H2 production system using an OHzS device powered by DHHPFC realizes hydrogen production at a stable rate (53.08 mol h−1 m−2). In-situ Raman tests and theoretical calculations unravel the metal-support interaction between Ir NPs and B, N-codoped porous carbon, optimizing the electronic structure and regulating the d-band center of Ir, reducing the adsorption energy of H* intermediates and N2H4 molecules, thus promoting the reaction processes of HER and HzOR.
Ultra-high nickel layered oxides are currently among the mainstream cathode materials for lithium-ion batteries (LIBs), having garnered extensive research and rapid development due to their high capacity. This review article defines ultra-high nickel oxides with a nickel content of ≥0.9 among transition metal components and proceeds based on this definition. Although high-nickel oxide cathode materials have undergone decades of development, the pursuit of increased capacity in ultra-high nickel oxides inevitably leads to compromised capacity retention, thermal stability, and unavoidable structural degradation, thereby hindering their progression. The review article focuses on summarizing the main challenges currently faced by ultra-high nickel oxides as cathode materials for lithium-ion batteries and as well as the mainstream modification measures. Finally, it is pointed out that the future research on ultra-high nickel oxides should focus on high-entropy modification, adaptation to extreme conditions, and the exploration of new preparation and modification methods. At the same time, efforts should be grounded in practical considerations and guided by target performance, aiming to improve various aspects of material performance for different application fields without compromising the high capacity inherent to ultra-high nickel oxide cathodes.
Coal tar (CT) has potential applications as a carbon material precursor due to its malleability and high carbon content. However, the low carbonization rate of CT is a major constraint to its development. In this work, a microporous carbon material (CF2CT) is synthesized from CT via the Friedel–Crafts alkylation reaction, which results in a significant increase in the carbonization yield (68%). In the absence of an activator, the CF2CT showed specific surface areas (766 m2 g−1) and micropore volumes (0.32 cm3 g−1), with pore diameters mainly centered on 0.5–0.8 nm. The CF2CT exhibited an excellent gravimetric capacitance of 342 F g−1 under 1 A g−1 in a three-electrode system, while its capacitance remained approximately 98% over 10 000 cycles under 10 A g−1. The symmetrical supercapacitors fabricated with CF2CT showed a 7.8 Wh kg−1 energy density and a 250 W kg−1 power density, with capacitance remaining up to 100% at 10 A g−1 after undergoing 10 000 cycles. This study proposes an idea for the preparation of high-yield carbon precursors from coal tar while also offering a promising HCP-derived carbon material for supercapacitor electrodes.
Among various electrode materials for supercapacitors, manganese oxide–carbon composites offer a promising balance of cost, performance, and environmental sustainability. Yet while these electrode structures can offer significant overall capacitance, the total capacitance is generally much lower than the theoretically achievable value, highlighting that the manganese oxide is in fact greatly underutilized. This study presents a novel one-pot metal-ammonia synthesis method for fabricating manganese oxide–activated carbon (MnAC) nanocomposites, designed to maximize manganese utilization in supercapacitor electrodes. By leveraging a thermodynamically driven deposition process, Mn3O4 nanoparticles are uniformly anchored onto activated carbon, overcoming limitations of conventional synthesis routes such as poor conductivity and underutilized active materials. The resulting MnAC composites exhibit high specific capacitance (120 F g−1) and 94% capacity retention after 1000 cycles, along with exceptional manganese efficiency (1044 F g−1 relative to Mn content), approaching theoretical limits. Structural and electrochemical analyses confirm the formation of a well-integrated, crystalline Mn3O4 phase with enhanced redox activity and conductivity. This scalable synthesis eliminates toxic solvents and enables ammonia recovery, offering a sustainable pathway for high-performance energy storage materials. The findings highlight the potential of MnAC composites for next-generation supercapacitors and establish a foundation for further optimization of metal oxide–carbon hybrid electrodes.
Molybdenum disulfide holds promise as a low cost and abundant catalyst for the hydrogen evolution reaction in an alkaline environment. However, its hydrogen evolution reaction activity is not sufficient for practical application because of its semiconducting properties in the 2H phase, presence of an electrochemically inert basal plane, and suboptimal hydrogen adsorption energy for hydrogen evolution reaction. In this article, we present a facile synthesis method for fabricating a Ni-doped molybdenum disulfide hydrogen evolution reaction electrode with a 1T structure through co-sputtering of molybdenum disulfide and Ni. Our results demonstrate that Ni doping not only promotes the 1T-phase yield in molybdenum disulfide structure but also activates the basal plane and improves the hydrogen adsorption energy of the edge plane. Also, the surface morphologies and 1T-phase yield, which are influenced by sputtering power and deposition time, are critical factors for the variation of hydrogen evolution reaction performance. Our Ni-doped molybdenum disulfide electrode, which exhibits high 1T yield and increased electrochemical surface area by tuning the morphology, shows an overpotential of ~91 mV at 10 mA cm−2, nearly 2.5 times lower than that of ~227 mV observed for molybdenum disulfide. Also, the single-cell test exhibits enhanced cell performance with improved durability in the repetitive on/off evaluation for the potential application of renewable energy integration.
Metallic copper nanoparticles are a promising alternative to gold and silver in printed electronics due to their excellent electrical and thermal conductivity. However, their synthesis is often hindered by rapid oxidation and limited scalability. This work presents a microwave-assisted polyol process for the rapid and scalable production of metallic Cu micro- and nanoparticles, performed in air without the need for an inert atmosphere. Ethylene glycol acts as both solvent and reducing agent, while lignin serves as a renewable capping agent. Reaction time is reduced to 10 min in batch mode, and the process is scaled up to a continuous-flow microwave system, achieving production rates of ~5 g h−1. Particle sizes range from 800 to 40 nm depending on lignin content and metal seeding. After pressure or low-temperature (150 °C) treatment, the materials reach conductivities between 30 and 100 μΩ·cm. These metallic copper nanoparticles show strong potential for use in sustainable conductive inks for flexible and printed electronics.
The oxygen evolution reaction suffers from sluggish kinetics and poor structural stability, necessitating the development of nonprecious metal electrocatalysts with efficient electronic regulation and intrinsic structural robustness. Herein, we construct a composite precatalyst of LaFe species modified cobalt carbonate hydroxide supported on nickel foam (LaFe–CoCH/NF) through a three-step process involving electrodeposition, hydrothermal growth, and co-deposition. This strategy enables the formation of a Ni–Co–Fe tri-level electron regulation pathway coupled with a spatially selective LaFe coating layer, achieving dual enhancement in both electronic modulation and structural stabilization. The hierarchical electron pathway effectively activates Ni sites within the nickel foam substrate, promotes the generation of high-valence Ni and Co species, and simultaneously suppresses the overoxidation of Fe. Meanwhile, the La-induced local electric field and buffering effect alleviate the detachment of the active phase during electrochemical reconstruction. As a result, the optimized LaFe–CoCH/NF catalyst exhibits outstanding oxygen evolution reaction performance, with a low Tafel slope of 33.75 mV dec−1 and exceptional durability, maintaining over 1500 h of stable operation at 10 mA cm−2, continuous operation for 1200 h at 50 and 100 mA cm−2, and more than 200 h of durability even at an ultrahigh current density of 500 mA cm−2. Mechanistic investigations reveal that the tri-metallic electron regulation strategy significantly improves interfacial charge transfer efficiency and structural integrity, offering theoretical guidance and a viable design route for advanced multi-metallic oxygen evolution reaction precatalysts.
Interfacial pH gradients significantly affect proton-coupled electron transfer (PCET) reactions, yet quantifying these dynamics under operando conditions remains challenging. Here, we present a dual-loop methodology that enables real-time, high-resolution mapping of interfacial pH fluctuations through probing hydrogen ion-specific adsorption potentials (HISAP). We effectively decouple electric field effects from genuine changes in proton activity, facilitating direct assessment of pH behavior across various electrolytes. Our results reveal that alkaline media can exhibit pH deviations over one unit at 100 mA cm−2, while buffered neutral systems display even greater gradients (ΔpH > 6) due to slow ion transport. By combining experimental data with Nernst-Planck models, we find that ion-specific mobility and buffer capacity are key to pH regulation. A 64% reduction in pH gradients occurs with increased buffer concentration, linking theoretical predictions with operando measurements. This reliable methodology spans the full pH range and high current densities, overcoming the limitations of traditional optical and probe-based techniques and providing a universal platform for understanding interfacial ion dynamics and optimizing electrocatalyst performance in energy conversion applications.
Cu3SbSe4-based compounds have attracted considerable potential in the realm of thermoelectric research owing to their distinctive physical properties and environmental compatibility. The material was efficiently synthesized via rapid microwave melting processing, aiming to improve its viability as a cost-effective thermoelectric option for practical applications. This study emphasizes the stepwise optimization of thermoelectric transport properties. The foremost effort involved improving transport electrical transport properties through the co-alloying of Sn and Te to determine optimal compositional configurations for superior thermoelectric performance. Iterative refinement enabled increased hole carrier concentration, which effectively addressed the intrinsic limitation of low electrical conductivity, thereby increasing the power factor by three times. Based on this foundation, a hierarchical multiscale structure was developed through the incorporation of AgCuTe as a secondary phase, which enhanced phonon scattering across multiple scales and consequently reduced thermal conductivity by 65% relative to pristine samples. The synergistic optimization of electronic and thermal transport properties culminated in a significant improvement in zT. The optimized Cu3SbSe4–1.0 wt% (Sn, Te)-2.5 wt% AgCuTe composite demonstrated a peak zT of 1.21 at 650 K and an average zTavg of 0.52 across the range of 300–650 K, contributing to a deeper understanding of the transport properties for chalcogenide-based thermoelectric compounds.
Boosting thermoelectric performance is challenging due to the intricate interplay between electrical and thermal transport properties. This study focuses on Zr vacancy-filled p-type Ti2Zr2Hf2Nb2Fe5.6Ni2.4Sb8-based thermoelectric materials to explore how Zr vacancies affect their structural and transport characteristics. Density functional theory calculations demonstrate that Zr vacancies induce proximal contraction/distal relaxation, strengthening lattice distortion while preserving the intrinsically intense phonon scattering in Ti2Zr2Hf2Nb2Fe5.6Ni2.4Sb8 samples. The intensified asymmetric electron localization between adjacent anions and the cation vacancies softens local chemical bonds. Microscopic investigations reveal that Ti2Zr2−xHf2Nb2Fe5.6Ni2.4Sb8 alloys with an optimal number of Zr vacancies balance the competing effects of carrier and phonon transport mechanisms by regulating multi-scale defects. Introducing appropriate Zr vacancies optimizes both the Seebeck coefficient and κL without greatly affecting electrical conductivity and weight mobility, achieving a 23% maximum power factor improvement and roughly 10% κL reduction. The bipolar diffusion effect is effectively suppressed to negligible levels by energy filtering effects, thus ensuring high-temperature stability. The maximum ZT of Ti2Zr1.97Hf2Nb2Fe5.6Ni2.4Sb8 and Ti2Zr1.95Hf2Nb2Fe5.6Ni2.4Sb8 is 30% higher than that of pristine samples without Zr vacancies. These findings are the first demonstration of vacancy engineering as a promising strategy in p-type double half-Heusler alloys to enhance their thermoelectric performance and decouple intertwined transport parameters.
Understanding the structural instability of high-voltage layered cathodes remains a critical challenge in advancing sodium-ion batteries. In particular, the mechanism of slab gliding, a key contributor to phase transitions, has not been fully elucidated at the atomic level. Here, we propose a breathing-shear mode coupling model based on the phonon spectrum, which elucidates the slab gliding mechanism in layered cathode materials by using interlayer spacing as the order parameter. Employing a “single-layer to double-layer” comparative strategy in P2-Na0MnO2, we establish a direct link between specific phonon modes and atomic-scale dynamics. This mode corresponds to a C-glide vibration, which features cooperative atomic motion within the layers and relative sliding between adjacent layers. Due to its negative vibrational energy, this mode drives exponential atomic displacement and triggers structural transformation. Notably, van der Waals-corrected phonon analysis reveals that weak interlayer interactions enhance this dynamic instability. Finally, we propose a solution to control structural stability by adjusting the interlayer spacing on the basis of phonon spectrum analysis. This phonon mode-stability correlation framework offers new theoretical guidance for designing robust high-voltage layered cathodes.
Ruthenium-based catalysts are promising alternatives to platinum for the hydrogen evolution reaction (HER) due to their comparable activity and lower cost. However, their widespread application in alkaline water electrolysis is limited by insufficient stability and excessive hydrogen binding. Herein, the Ru@Co3O4 nanosheets (Ru@Co3O4 NSs) featuring dominant exposure of the Co3O4 (111) facets and precise anchoring of Ru nanoclusters onto these planes were constructed. The interaction between Ru nanoclusters and the Co3O4 (111) facets induces a downshift of the Ru d-band center, optimizes the interfacial water network, and simultaneously prevents the leaching of Ru species. Ru@Co3O4 NSs deliver exceptional alkaline HER performance, with an overpotential of 9.8 mV at 10 mA cm−2 and robust durability over 1000 h at 1 A cm−2. The catalyst also achieves a price-normalized activity of 145.9 A $−1, nearly nine times that of commercial Pt/C. When applied in an anion exchange membrane water electrolyzer (AEMWE), Ru@Co3O4 NSs reveal a low cell voltage of 1.93 V at 1 A cm−2 and operate stably for 60 h with a minimal degradation rate of 0.67 mV h−1. This work provides a promising approach for designing low-cost, high-performance Ru-based catalysts for sustainable hydrogen production.
Lithium–sulfur (Li–S) batteries hold tremendous promise for next-generation energy storage due to their high theoretical energy density and low cost. However, commercialization is hindered by severe polysulfide shuttling, sluggish redox kinetics, and rapid capacity decay under practical loading conditions. Herein, we report a rationally engineered SnSe2@Ti3C2Tx MXene heterostructure as a multifunctional separator coating that synergistically combines strong Lewis acidic adsorption sites with catalytic interfaces and a highly conductive, polar-terminated MXene matrix. The SnSe2 nanosheets provide abundant catalytic centers to accelerate the redox conversion of soluble Li2Sx species, while Ti3C2Tx ensures rapid electron transport and robust chemical immobilization of polysulfide intermediates. This interfacial synergy effectively suppresses the shuttle effect, lowers electrochemical polarization, and promotes rapid charge transfer. Electrochemical evaluations reveal an initial discharge capacity of 1626 mAh g−1 at 0.2 C with nearly 100% Coulombic efficiency. Under high sulfur loading (5 mg cm−2) and lean-electrolyte conditions (E/S = 6 μL mg−1), cells with the SnSe2@MXene-coated separator deliver 751 mAh g−1 after 120 cycles, retaining 70.9% of their initial capacity. Remarkably, long-term cycling at 1 C exceeds 1000 cycles with 44.4% capacity retention and minimal structural degradation. This work demonstrates a scalable, effective separator-engineering strategy, establishing SnSe2@MXene as a promising platform for practical, high-energy-density Li–S batteries.
The antagonism between porosity and graphitization critically limits carbon supercapacitor performance. Here, we demonstrate a structural engineering strategy that converts Sargentodoxa Cuneata residue (SCR) into hierarchically porous graphitic carbons (SCR-HPCs). By precisely regulating biomass precursor porous architecture, this methodology decouples the antagonism between porosity development and graphitization progression in KOH-mediated activation, achieving simultaneous high specific surface area (2465.1 m2 g−1) and graphitization (ID/IG of 0.73). In 6 m KOH electrolyte, the specific capacitance of the optimized SCR-HPC-900 electrode reaches 415.6 F g−1 at 0.5 A g−1, with a capacitance retention of 75.1% even at an ultra-high current density of 200 A g−1. The fabricated symmetric supercapacitor achieves an energy density of 8.5 Wh kg−1 at a power density of 37 803 W kg−1, retaining over 100.8% of its capacitance after 100 000 cycles. Remarkably, in 1 m TEABF4/PC organic electrolyte, the supercapacitor achieves maximum energy and power densities of 45.6 Wh kg−1 and 41 750 W kg−1, respectively. This study presents an effective methodology for decoupling the antagonism between porosity and graphitization in conventional processes, offering a new idea for converting biomass waste into high-performance energy storage materials.
Aqueous zinc metal batteries (AZMBs) are considered ideal ones for next-generation energy storage devices due to their high theoretical specific capacity and intrinsic safety. However, uncontrollable zinc dendrite growth, hydrogen evolution reaction (HER), and interface corrosion prohibit the commercialization of AZMBs. The deposition behaviors of Zn2+/Zn0 on metallic Zn surface can be effectively regulated by constructing artificial interphase layers (AILs) to control desolvation and ion/atom flux. In this work, the intrinsic mechanism and interface failure of Zn2+ electrodeposition behaviors are initially revealed, providing a theoretical basis for interface issues. To address these problems, the design strategies from carbon materials, zincophilic alloys, and inorganic/organic compound layers provide an in-depth analysis of the relationship between material structure and performance, establishing a theoretical foundation for the development of programmable interface architecture. In light of practical application requirements, the future direction is envisioned and pioneered, aiming to promote the practical application process of AZMBs.
Photocatalytic CO2 fixation into value-added chemicals can not only mitigate the greenhouse effect but also alleviate the energy crisis. In the field of photocatalytic CO2 reduction, copper-based photocatalysts have been intensively studied for producing value-added multi-carbon (C2+) products. In view of this, noncopper-based photocatalysts under visible light irradiation are summarized and reviewed herein. First, the principles on how to realize C–C coupling on photocatalysts' surfaces are discussed. In the following, different strategies for making photocatalysts to absorb visible light and enable C–C coupling, including alloying, layered structures, single atoms, forming spinel structures, and so on, are outlined and discussed. In order to materialize visible light utilization and C–C coupling, the advantages and disadvantages of these strategies are commented. To conclude, we provide insights into the prospects and potential advancements for the visible-light-driven CO2 conversion to C2+ products.
The spatial resolution of X-ray imaging is often limited by radioluminescence scattering, which is exacerbated in thick scintillators and unpatterned films due to lateral light spreading. Commercial scintillators such as cesium iodide and gadolinium oxysulfide, although hundreds of micrometers thick to ensure efficient X-ray absorption, still suffer from optical crosstalk, complicated fabrication, and high production costs. To overcome these challenges, we report a novel micropatterned lead-free green and sustainable 1D Cu-based perovskite nanocrystals scintillator film. Specifically, polyethylene glycol-coated CsCu2I3 nanocrystals are used to achieve improved quantum yield and precise thickness control, facilitated by the flexibility and compatibility of polyethylene glycol with the Cu-based nanocrystals. During polyethylene glycol treatment, zero-dimensional Cs3Cu2I5 nanocrystals transform into 1D CsCu2I3 nanocrystals, occurring, accompanied by a pronounced redshift in emission, enabling the fabrication of yellow-emitting scintillator films. Further, photolithographic techniques are used to fabricate patterned substrates with varying pattern sizes and thicknesses, which were subsequently filled with polyethylene glycol-coated CsCu2I3 nanocrystals via a hot-press method. The optimized micropatterned scintillator film effectively suppressed optical crosstalk and delivered enhanced spatial resolution under a clinically relevant tube voltage (80 kVp), outperforming unpatterned counterparts. X-ray imaging at such high voltage conditions has rarely been demonstrated using copper halide materials. This strategy highlights a practical route toward clinically relevant, scalable, and high-resolution scintillator films for advanced X-ray imaging.