Nitrogen-doped carbon aerogel materials exhibit significant potential as catalysts for the oxygen reduction reaction (ORR) in fuel cell applications. However, their widespread application is hindered by complex synthesis, high cost, and small pore size. Herein, we report a facile one-step carbonization method to synthesize a mesoporous nitrogen-doped carbon aerogel using phloroglucinol, resorcinol, and formaldehyde as raw materials, coupled with melamine doping. This carbon aerogel exhibits a controlled and uniform defect distribution (nitrogen doping:1.93 %), a high graphitization degree (ID/IG = 0.83), a large pore size (10-20 nm), and remarkable hydrophilicity (water contact angle = 16 degrees). These distinctive structures synergistically enhance a resistance to methanol poisoning, with a retention rate 1.95 times that of the undoped sample. They also improve the ORR catalytic performance, yielding 1.66 times higher mass activity than the undoped counterpart. This design offers a novel approach to the mass production of mesoporous nitrogen-doped carbon aerogel, which has great application potential and economic benefit as a catalyst.
The practical deployment of silicon (Si) anodes is limited by coupled mechanical failure and sluggish electrochemical kinetics arising from repeated volume expansion. While polymer binders are critical to electrode integrity, conventional designs often prioritize mechanical strength over ion transport. Here, a supratopological ion-coordinated binder (PVA-AA-5SAS) by integrating a hyperbranched PVA-AA framework with the sulfonated aromatic small molecule 5-sulfoisophthalic acid sodium salt (SAS) via in situ esterification is developed. The resulting 3D network effectively suppresses polymer chain slippage while simultaneously forming continuous Li+-coordination pathways via cooperative interactions between ester and sulfonate groups. This dual-function architecture markedly accelerates Li+ diffusion, reduces charge-transfer and SEI resistances, and stabilizes interfacial chemistry during deep lithiation. Si electrodes employing this binder demonstrate excellent rate capability and long-term cycling stability, maintaining a capacity retention of 79.2% after 386 cycles at 1 A in a 1 Ah‑level NCM811//SiC550 pouch cell. These results demonstrate that rational binder design can decouple and resolve the long-standing conflict between structural durability and ion conduction, providing a viable route toward kinetically efficient and mechanically durable Si-based batteries.
Solar-driven interfacial evaporation technology holds significant potential, as evaporation-induced hydropower generation can directly convert ambient thermal energy into electrical energy, thereby addressing both freshwater scarcity and the global energy crisis. In this study, a hydrogel-based solar interfacial evaporator-comprising carboxymethyl cellulose (CMC), cellulose nanofibers (CNF), carbon nanotubes (CNT), and polypyrrole (PPy) integrated within a polyacrylamide (PAM) matrix-is developed using Pickering emulsion polymerization. The system leverages nanofibrillar cellulose-assisted CNT and PPy as emulsion stabilizers to effectively tackle the dual challenge of freshwater production and electricity generation. The resulting MFTP-PAM hydrogel evaporator exhibits enhanced light absorption and photothermal conversion efficiency, enabling concurrent solar-driven water evaporation and thermoelectric power generation. Under one sun irradiation, the optimized evaporator achieves a high evaporation rate of 1.53 kg m-2 h-1 in tap water and generates an output voltage of 470 mV in a 3.5 wt% NaCl solution. Furthermore, the MFTP-PAM hydrogel evaporator can desalinate and prevent contamination. This study aims to propose a simple and reliable modification method to enhance the evaporation performance of Pickering-based hydrogel evaporators and to improve their hydrogel network structure to produce both clean water and electricity, which is a promising energy solution.
Lithium cobalt oxide (LCO) is a typical layered structure cathode material for high-energy-density lithium-ion batteries. However, its structural instability at high voltages limits the operational voltage window in practical applications. In this study, a water-soluble composite binder, poly(acrylamide-co-acrylonitrile)-carrageenan (PMN-CRN), was designed and synthesized for application in high-voltage cathodes. The binder consists of PMN, a water-soluble polymer produced by copolymerizing acrylamide (AM) and acrylonitrile (AN), and lambda-carrageenan (CRN), a natural polysaccharide enriched with sulfate groups, which are blended to build a 3D cross-linked network structure through hydrogen-bonding interactions. This structure is suitable for electrode slurry processing and stabilizing the interface construction. The PMN-CRN enhances the stability of the cathode solid electrolyte interface (CEI) and effectively inhibits the structural collapse and irreversible phase transitions at high voltages, thereby improving the interfacial stability and cycling durability of the electrodes. The capacity retention rate of LCO@PMN-CRN reaches 94.6% after 200 cycles at 1C, and maintains a reversible capacity of approximately 150 mAh g-1 at 5C. The outstanding electrochemical performance indicates that the PMN-CRN binder effectively stabilizes 4.6 V LCO cathode, which has the potential to be applied to high-energy-density lithium-ion batteries.
Lithium cobalt oxide (LCO) is a prominent cathode material for lithium-ion batteries. However, its application at high voltages (> 4.45 V) is hindered by detrimental side reactions, including the dissolution of high-valence cobalt (Co4+) and the release of lattice oxygen. To address these challenges, we developed a novel cyanoethyl-functionalized binder, cyanoethyl chitosan (CSAN), derived from the natural biopolymer cationic chitosan (CS). The introduced cyanoethyl groups markedly enhance the polymer's polarity and coordination strength. This dual functionality not only facilitates rapid Li+ transport but also effectively chelates cobalt ions, thereby suppressing their dissolution from the lattice. The synergistic effect of these actions significantly improves the ionic conductivity and structural integrity of the cathode, leading to substantially enhanced capacity retention and cycling stability under high-rate conditions. When evaluated in LCO half-cells at 4.6 V, the CSAN binder enabled exceptional long-term cycling stability and rate performance. The cell retained 73% of its capacity after 1000 cycles at 1C and delivered a capacity exceeding 100 mAh g(-1) even at 10C. This work underscores the significant potential of functionalized biomass-derived binders for enabling high-voltage, high-energy-density LCO cathodes.
Au-doped lithium hydride (LiH) demonstrates significant potential for applications in advanced energy storage systems and radiation absorption. However, due to the large density difference between gold (Au) and LiH, achieving uniform dispersion of Au remains a significant challenge, which hinders the development of Au-doped LiH. Herein, we report a method for achieving uniform Au dispersion. Using LiH as the raw material and parylene as the pore-forming agent, together with Au doping, we successfully synthesized Au-doped foamed LiH. This material has a highly porous structure with uniformly distributed Au particles, with a predominant particle size of 1.7 μm. Discrete element simulation also confirms that small Au particles around LiH achieve the highest uniformity. This material enables a novel synthetic route to metal-doped LiH and offers considerable promise as a dual-functional material for hydrogen storage and radiation shielding.
Cathode chemistries directly dictate the energy densities of advanced batteries; however, these chemistries of high voltage and high capacity present a severe challenge to the reversibility of the batteries, incurring irreversible reactions between electrolytes and cathodes, resulting in electrolyte and lithium inventory consumption as well as interfacial degradation of cathode lattice structures. Here, departing from the conventional approach of electrolyte engineering, we report that the polymeric binder, an often-overlooked ingredient in the electrode composite, can mitigate all these parasitic reactions in a more economical and effective manner. The lignin-functionalized polymonofluoroacrylic acid (PFA) was shown to stabilize a wide spectrum of aggressive cathode chemistries, including LiNi0.8Co0.1Mn0.1O2 (NCM811), LiCoO2 (LCO), and 5-V class LiNi0.5Mn1.5O4 (LNMO), with superior performances. Besides providing robust adhesive force to keep the active and conductive ingredients within the cathode composite in intimate contact, especially when the cathode experiences extreme mechanical and electrochemical stress under high voltages, PFA also serves as an F source to form LiF-rich interphases on cathode materials that insulate parasitic reactions with electrolytes. Lignin, on the other hand, makes PFA well-dispersed in the cathode composite, rendering it with excellent radical-scavenging ability. Altogether, the lignin-PFA binder combination proves versatile in stabilizing these cathodes in both lithium-ion and lithium-metal configurations, enabling the Li||NCM811 cell to maintain 77% capacity after 500 cycles at 4.6 V, or a 2.2 Ah graphite||NCM811 pouch cell with 91.2% capacity retention after 500 cycles at the high cutoff voltage of 4.6 V. This molecular design approach for an advanced binder offers a completely different and unique route to increase the energy densities of advanced batteries.
Silicon-based anodes are promising for high-energy-density lithium-ion batteries but suffer from severe volume expansion and interfacial instability. Herein, a fluorine-substituted unsaturated phosphate ester additive (PEFA-3) is proposed to address these challenges. The PEFA-3 exhibits tailored electronic properties and a low electrostatic potential difference, enabling its preferential oxidation at the cathode and reduction at the anode. This behavior facilitates the formation of robust, polyyne network enhanced interphases (SEI/CEI) on both electrodes. In the 1.6 Ah NCM811||S600 pouch cells, PEFA-3 enhances cycling stability by achieving 94.6% capacity retention after 300 cycles with the average Coulombic efficiency >99.9%, while effectively suppressing gas evolution and silicon-based anode failure. The Liquid Chromatography-Quadrupole Time-of-Flight Mass Spectrometry (LC-QTof-MS) decouples the decomposition pathways of PEFA-3 at the electrodes, which indicates that crucial species such as C6H8O4F3P in SEI/CEI are beneficial for reinforcing interfacial integrity and inhibiting electrolyte degradation. Our design concept for electrolyte additives provides a promising path to silicon-based energy-dense lithium-ion batteries.
Polyethylene separators (PE) are widely used in lithium-ion batteries due to their good electrochemical stability and low cost. However, PE separators have issues including high-temperature shrinkage and poor electrolyte wettability, which reduce the safety and electrochemical performance of batteries. In this work, we synthesized a large-sized microsphere binder (SNE) and designed an inorganic ceramic/polymer composite coating strategy. The prepared single-layer PE/SNE separator exhibits a unique micro-convex structure, where microspheres with diameters slightly larger than the thickness of the ceramic layer are partially exposed outside the composite coating. The electrodes and separators are hot-pressed to make the microspheres viscoelastic, which effectively bonds the electrodes, prevents sliding, and strengthens the interface to reduce interface impedance. Compared to traditional PVDF-coated ceramic separators, PE/SNE separators feature simple production processes, lower cost, and environmental friendliness. The ceramic-coated optimized PE/SNE separator can maintain shrinkage of <1% at 130 degrees C/0.5 h and improves the ionic conductivity (0.83 mS/cm) and lithium-ion transference number (t(Li)(+) = 0.62). Due to the optimized hot-pressed interface and improved overall performance of the PE/SNE separator, the NCM622//Li cell has a discharge capacity of 118 mAh/g at 5C, and the NCM622//graphite full cell has a capacity retention rate of 81% after stable cycling for 1500 cycles at 2C. This approach offers a promising method for developing lithium-ion battery separators with enhanced safety and cycling performance.
Lithium-sulfur (Li-S) batteries have garnered increasing attentions due to their ultrahigh energy density. However, their practical applications are significantly impeded by the shuttle effect of polysulfides, the corrosion of lithium anodes, and the formation of lithium dendrites. Here, we design a dual-function cottonseed proteinbased separator coating (Mn-P-CPI) by synchronously grafting phosphate groups and metalloporphyrin compounds, which is capable of adsorbing and catalyzing polysulfides. As such, the assembled Li-S battery not only exhibits much-improved specific capacity (up to 983.5 mAh g- 1 at 1C), but also maintains high cycling stability (the capacity attenuation is only 0.066% per cycle). More notably, Mn-P-CPI can serve as the binder of cathode electrode benefiting from its abundant active groups. By simultaneously employing Mn-P-CPI as electrode binder and separator coating, the battery displays a high specific capacity (752.8 mAh g- 1 at 0.5C) under 2.11 mg cm- 2 of sulfur loading and the exceptional rate performances (719.3 mAh g- 1 at 3C). This strategy offers a promising alternative to develop a high-performance separator coating for Li-S batteries, as well as opens up a feasible way for realizing the application of biomass materials in the field of energy storage.
The global challenges of freshwater scarcity and sustainable energy demand drive the development of integrated systems capable of concurrent solar desalination and electricity generation. We present a dual-asymmetric PVA/cellulose/CNT composite hydrogel synthesized via Pickering emulsion templating and freeze-thaw cycling. This design constructs a gradient porous network with continuous wettability and charge-density gradients by using CNF and CMC as structural and physicochemical modifiers. The dual asymmetry arises from the gradient porous architecture stabilized by CNF and CMC emulsions, as well as the continuous wettability and charge gradient derived from differing hydrophilicity and zeta potential between CNF and CMC. The incorporated CNTs act as efficient photothermal conversion agents, giving the hydrogel a broadband solar absorption efficiency of similar to 98%. Under 1-sun irradiation, the optimized hydrogel achieves an evaporation rate of 1.21 kg m(-2) h(-1) for tap water and 0.95 kg m(-2) h(-1) for 3.5 wt % NaCl solution, while generating an open-circuit voltage up to 440 mV in saline and 470 mV in acidic solutions. The dual-asymmetric structure significantly enhances hydrovoltaic output by synergistically regulating ion transport and charge accumulation. This work provides a rational design for multifunctional hydrogel evaporators, offering a sustainable route for decentralized water and energy co-generation.
Due to the large specific surface area and abundant active sites, the metal organic frameworks (MOFs) have been widely considered as the promising electrode materials for supercapacitors (SCs). In this work, the Co-MOF nanosheets (NSs) were deposited onto carbon cloth (CC) using a simple, binder-free electrodeposition method. The morphology and surface composition of Co-MOF NSs were modified by a hydrothermal treatment in a nickel nitrate aqueous solution. The modified Co-MOF electrode exhibited outstanding electrochemical performance for supercapacitor application, delivering the large specific capacitance of 1344.0 F g-1 at 1 A g-1 in a three-electrode system, good rate capacity and good stability during the cyclic test. The charge storage of the Ni2+-modified Co-MOF was generally dominated by the pseudocapacitance mechanism. The asymmetric supercapacitor (ASC) devices were assembled by using the Ni2+-modified Co-MOF as the cathode and activated carbon (AC) as the anode. The ASC devices also displayed competitive electrochemical performance, achieving an energy density of 43.4 Wh kg-1 at the power density of 850.0 W kg-1. The findings highlight the potential application of Ni2+-modified Co-MOF nanosheets for supercapacitor. The research also provides a universal route to regulate the microstructure and composition of the Co-MOF based electrodes.
This review comprehensively summarizes the latest advancements in the synthesis and multifaceted applications of metal-organic frameworks (MOFs) for clean water. It systematically explores scalable synthesis methods, from solvothermal to green mechanochemical routes, and highlights the innovative transformation of waste into high-value MOFs. The article delves into the diverse functionalities of MOFs in water remediation, including the adsorptive and catalytic removal of heavy metals, organic pollutants, pharmaceuticals, PFASs, and micro/nano-plastics. Applications in sensing, radionuclide separation, oil-water separation, and advanced membrane technologies are also detailed. Furthermore, emerging roles in water capture, algal inhibition and resource recovery are discussed. Finally, the review provides a critical perspective on future challenges and opportunities, emphasizing sustainable synthesis, life-cycle assessment, and the integration of AI for the intelligent design of next-generation MOFs, paving the way for their transition from laboratory research to real-world water treatment solutions.
Flexible lithium metal batteries (LMBs) using polymer-based solid-state electrolytes (PSSEs) are highly desirable for wearable applications because of the potential advantages in energy density and safety. Recently, ether-based polyelectrolytes have received extensive attention because of their good stability, high ionic conductivity, and Li metal anode compatibility. However, it typically forms organic-rich cathode electrolyte interphase (CEI) at the cathode, which is still a pain point that impedes the high-voltage performance. To address this challenge, herein a fluorinated plasticizer, bis(2-fluoroethyl) ether (BFE) is reported, which can be easily blended into ether-based PSSE and enables high-voltage-stable flexible LMBs. The BFE and PSSE molecules form an atypical hydrogen bond interaction, which weakens the interaction between PSSE and lithium ions. This leads to the formation of an anion-rich solvation structure that generates inorganic-rich and high-voltage-stable CEI. The oxidation stability of PSSE is improved from 4.4 V to over 4.7 V after introducing the BFE molecules. LMBs using BFE-blended PSSE can couple with high-voltage cathode and retain 80% capacity after 480 cycles at 1C. Full cells show high energy density (752.2 Wh L-1) outstanding capacity retention per cycle (99.88%), and high flexibility with almost identic charge/discharge characteristics after 4000 bending cycles.
Solid-state electrolyte (SSE) is a potential way to solve the safety problems of lithium metal batteries (LMBs), and Li6.5La3Zr1.5Ta0.5O12 (LLZTO) is one of the most extensive research SSEs due to its good air stability and wide electrochemical window. However, the residual alkali on LLZTO surface limits its application with polyvinylidene difluoride (PVDF)-contained binders, and the uncontrollable lithium dendrites growing between the grain boundaries of LLZTO particles would lead to rapid capacity fading and potential short circuit risk. Herein, by in situ coating Li3PO4 (LPO) on LLZTO particles (LLZTO@LPO) evenly, the residual alkali on the LLZTO surface is neutralized and the pH value is reduced to 8.84. The modified LLZTO can be mixed with PVDF solution and shows good fluidity without a cross-linking reaction, making the subsequent ceramic coating on the separator feasible. The LLZTO@LPO coating polyethylene (PE) separator can achieve 1400 h (115% increase) stable cycling under 1 mA cm(-2) current density in the Li parallel to Li symmetrical cell and 80% capacity retention after 260 cycles (NCM622-Li coin cell with 3 mAh cm(-2) loading). Furthermore, the LLZTO SSE pellets were prepared with the LLZTO@LPO and assembled in coin cell. The critical current density (CCD) result increases from 0.7 to 1.6 mA cm(-2) owing to that the LPO coating effectively inhibits the lithium dendrites formation through LLZTO grain boundaries. This work provides a strategy for fabricating the coating layer on LLZTO to improve the stability of LMBs.
The silicon microparticles (SiMPs) offer a promising solution for high‐energy‐density lithium‐ion battery systems. However, the inevitable volume expansion (>300%) of SiMPs during alloying often leads to particle breakage, interface rupture, and electrode separation, resulting in rapid capacity decay. Herein, an effective strategy is proposed for designing a novel solid–liquid hybrid electrode (Si@EGaSn) for high‐energy‐density flexible lithium‐ion batteries. The Si@EGaSn electrode has a liquid‐phase top layer containing SiMPs and a solid‐phase copper gallium alloy bottom layer. The top layer can not only electrically connect the fractured SiMPs, but also form a stable solid electrolyte interface during alloying processes. The bottom layer can firmly adhere the electrodes to the current collector. Consequently, the optimal Si@EGaSn electrode delivers a highly reversible capacity of 767.1 mAh g −1 at 0.5 A g −1 and a high capacity retention of >99% during 200 cycles. After loading the electrode into metallic textiles, the assembled high‐voltage pouch cell of NCM811//Si@EGaSn shows a high areal capacity of 3.2 mAh cm −2 , high volumetric energy density of 500 Wh L −1 and negligible capacity decay during 3000 flexing cycles at a small bending radius of 4.0 mm. This work provides a new electrode design approach to achieve high‐energy‐density flexible lithium‐ion batteries.
The growing concerns regarding the ecological and human health risks posed by ofloxacin (OFC) contamination have intensified the demand for advanced multifunctional materials to address antibiotic pollution in wastewater. In this study, a europium(III) functionalized metal-organic framework (Eu@MOF-303) was developed as dual-functional platform for adsorption and fluorescence-based detection of OFC. Through post-synthetic modification, Eu3+ ions were anchored onto MOF-303 ' s porous structure, serving as chelating centers for target capture and luminescent signal transduction. The Eu@MOF-303 demonstrated exceptional OFC adsorption capacity of 1688.66 mg center dot g-1, attributed to its high surface area (916.32 m2 center dot g-1), favorable surface charge (68.01 mV), and abundant Eu3+-derived active sites. Mechanistic studies revealed that synergistic interactions-including hydrogen bonding, it-it stacking, and coordination bonding-governed the adsorption process. Furthermore, Eu@MOF-303 exhibited unique fluorescence properties with characteristic red emission at 615 nm, enabling selective OFC detection via a static quenching mechanism. The Eu@MOF-303 achieved a low detection limit of 3.27 mu M across a wide linear range (0-200 mu M), while maintaining remarkable selectivity towards quinolone antibiotics. Notably, the OFC-saturated adsorbent displayed enhanced antibacterial activity, suggesting secondary utility in microbial control. This study presents a pioneering strategy for designing intelligent materials that integrate pollutant removal, environmental monitoring, and antibacterial ability as a versatile solution for sustainable wastewater remediation.
Lithium iron phosphate/graphite (LFP/Gr) batteries are widely recognized for their excellent safety performance; however, their practical application under low-temperature and fast-charging conditions remains challenging due to sluggish lithium-ion interfacial dynamics. In this work, a nitrile-based electrolyte containing N,N-dimethyltrifluoroacetamide (FDMA) is reported, which modulates lithium-ion solvation through hydrogen bonding with the nitrile solvent (IBN), thereby optimizing interfacial transport and stabilizing the solid electrolyte interphase (SEI) at low temperatures. The Ah-level LFP/Gr batteries with this electrolyte demonstrate outstanding cycling stability, maintaining 99.9% capacity retention over 800 cycles at -20 degrees C. Furthermore, the electrolyte delivers a discharge capacity of 759 mAh at -40 degrees C, more than three times higher than that of the baseline EC/DEC electrolyte. At room temperature, the pouch cells sustain 80% capacity retention after 535 cycles at a 2C fast-charging rate with an average coulombic efficiency of 99.9%. This electrolyte design, driven by hydrogen-bond-regulated solvation structure, significantly enhances low-temperature performance and cycling stability while maintaining excellent stability at room and elevated temperatures. These findings provide valuable insights for developing next-generation electrolytes aimed at lithium-ion batteries operating under extreme conditions.
Polycyclic aromatic hydrocarbons (PAHs), especially pyrene, are hazardous pollutants with serious health risks. Effective detection methods for PAHs are essential for environmental monitoring. In this study, we construct a simple, efficient method to detect pyrene derivatives in water. A squaraine dye (J3-Ad) with dual host-guest sites was synthesized and paired with a β-cyclodextrin dimer (H2-CD) to regulate host-guest interactions. In the presence of pyrenes, J3-Ad monomers in the J3-Ad/H2-CD mixture (JH-AC) are displaced by pyrenes and self-assemble into H-aggregates, resulting in a ∼135 nm absorption spectral shift. The transformation was confirmed through Scanning Electron Microscope (SEM), Dynamic Light Scattering (DLS), and Density Functional Theory (DFT) analysis. The system showed high sensitivity, with detection limits of 1.76 nmol/L for pyrene and 60.02 nmol/L for 1-hydroxypyrene (1-OHP), along with strong anti-interference and reliable colorimetric recognition. A smartphone-based, real-time detection platform was developed for visual monitoring of pyrene in soil and vegetables. Pyrene in tap water and river water, as well as 1-OHP in urine, were successfully detected, with acceptable recovery rates and a relative standard deviation (RSD) of less than 10.14 %. This work provides a sensitive, rapid, and visual method for tracking PAH pollution, offering significant potential for practical, on-site environmental applications.