Superhydrophobic coatings hold immense potential in anti-icing applications. The preparation of superhydrophobic anti-icing coatings involves multi-parameter design such as coating components and substrate structures, which leads to high trial-and-error rates and unclear directionality in performance optimization. Here, we first report a full-process machine learning framework that integrates large language model, post-hoc explainable machine learning model, and Bayesian Optimization framework to guide the preparation of superhydrophobic coating with superior anti-icing performance. The FPMLF autonomously collected 217 sets of coating components data from 2315 published articles, constructed a regression model for coating components design based on the collected data, and achieved the high throughput screening and optimization of the complex process parameters of the substrate structure. Guided by this framework, we successfully fabricated a coating exhibiting a freezing delay time over 30-fold longer than bare substrate. This work provides systematic support and a methodological foundation for the rational design of advanced functional materials with coupled and complex performance requirements.
To address the critical bottlenecks of weak coating adhesion, reliance on fluorinated reagents/organic solvents, and insufficient durability in superhydrophobic modification of cement-based materials, this study proposes an eco-friendly monolithic modification strategy based on molecular template-guided sol-gel assembly. Using water as the sole solvent, polyvinyl alcohol acts as a green molecular template, synergizing with octyltriethoxysilane, tetraethyl orthosilicate, and dual-scale SiO2 nanoparticles (30 nm/200 nm). The alkaline cement hydration environment triggers in-situ hydrolysis, condensation and assembly, constructing an organic-inorganic hybrid hierarchical micro/nano-rough structure throughout the monolithic mortar. The modified superhydrophobic cement mortar (SNC) achieves a water contact angle of 152 degrees+0.5 degrees and a sliding angle of 5 degrees+0.5 degrees, and maintains stable superhydrophobicity under various sandpaper abrasion tests owing to its abrasion-induced dynamic renewal mechanism. After 40 days of immersion in acidic, alkaline or salt solutions, its water absorption is reduced by more than 72% compared with ordinary mortar (ONC). The SNC sample can withstand 200 freezethaw cycles, and exhibits excellent resistance to UV radiation and thermal shock. Electrochemical tests show that the corrosion current density of embedded iron nails in 3.5 wt% NaCl solution is about five orders of magnitude lower in SNC than in ONC after 1 day of immersion, and remains four orders lower even after 30 days. This method avoids harmful fluorinated reagents and organic solvents, realizes true monolithic functionalization, and breaks through the limitations of traditional modification. It provides a novel route for preparing durable and eco-friendly superhydrophobic cement-based materials, and is of great significance for improving the waterproofing, anti-corrosion and long-term durability of infrastructure.
MnO2 has emerged as a promising electrode material for aqueous ammonium ion supercapacitors due to its low cost and high theoretical capacitance. However, its practical application is hindered by inherently low electrical conductivity, insufficient practical capacitance, and poor structural stability during cycling. Herein, a synergistic optimization strategy is developed via intralayer and interlayer Mo/NH4+ dual-ion pre-intercalation. Intralayer Mo-doping modulates the microstructure and crystal structure of MnO2, increases active sites, and enhances conductivity through the introduction of oxygen vacancies. Meanwhile, in-situ electrochemical activation is employed to pre-intercalate NH4+ ions, which further elevates the oxygen vacancy concentration and significantly improves the structural stability of the material. The optimized Mo-MnO2/AC electrode delivers a high specific capacitance of 668.5 F g-1 at 2 mA cm-2 and retains 97.92
Ternary metal sulfide (ZnIn2S4) is a promising photoanode material for photoelectrochemical (PEC) applications, yet its performance suffers from intrinsically low charge mobility and high defect density. Introducing oxygen (O)-related defects can improve carrier concentration and suppress recombination, but conventional air annealing lacks precise control over O incorporation. Here, we report an antimony (Sb)-induced defect and surface homojunction engineering strategy for ZnIn2S4 using a simple spin-coating and annealing process. Sb incorporation increases the content of O-related shallow-level donor states, which improves carrier concentration and mitigates defect-related recombination. Moreover, the surface-enriched Sb and O form a favorable surface/bulk homojunction with the intrinsic ZnIn2S4 interior, facilitating efficient carrier separation and transport. As a result, the optimized photoanode delivers an impressive photocurrent density of 4.30 mA cm-2 at 1.23 V versus the reversible hydrogen electrode (V vs. RHE) and a maximum applied bias photon-to-current efficiency (ABPE) of 2.00% in 0.5 M Na2SO4 electrolyte under AM 1.5G illumination, representing the highest reported value for ZnIn2S4-based photoanodes in neutral electrolyte without sacrificial agents. These findings highlight a promising defect engineering strategy to improve PEC performance of ternary metal chalcogenides.
Superhydrophobic coatings have been considered as promising candidates for anti-icing application in recent years. However, such coatings are easily damaged by mechanical loads due to their fragile micro/nanostructures, and they are also prone to transit from the Cassie-Baxter to the Wenzel state during icing process, which greatly limits their lifespan. Herein, a superhydrophobic coating with a water contact angle of 152.5(degrees) and water sliding angle of 4(degrees) was prepared on aluminum substrate through chemical etching followed by spinning. The coating possesses high-aspect-ratio micro-protrusions and strong interlock with substrate, thereby endowing it with a larger energy barrier for water impaling in rough structure, smaller heat losses with freezing droplet, superior protecting effect for nanostructure. Consequently, the coating exhibits enhanced anti-icing and mechanical robustness with a similar to 7.7-fold prolongation in freezing delay than the bare Al substrate and superior withstanding capacity in a series of tests. It can be expected that the coating has a promising prospect in the practical anti-icing applications owing to its straightforward fabrication, good mechanical robustness and excellent anti-icing property.
Sb-induced O-related defect engineering promotes lattice/near-lattice oxygen incorporation and a surface/bulk homojunction in ZnIn 2 S 4 , thereby enhancing charge separation and improving PEC activity under anodic operation.
Addressing the high energy consumption and greenhouse gas emissions associated with conventional active cooling technologies, daytime passive radiative cooling has attracted significant interest due to its zero-energy cooling characteristics. However, its practical application remains challenging due to the difficulty in balancing optical performance, fabrication cost, process complexity, and environmental durability within existing material systems. This study utilizes industrially derived alpha-hemihydrate phosphogypsum (alpha-HPG) as a functional inorganic filler to develop an SPG-DM0.6S composite coating with integrated cooling performance, superhydrophobicity, and self-healing capability through hydrophobic group grafting and compounding with polymethyl methacrylate (PMMA). Experimental results demonstrate that the coating achieves an average temperature reduction of 19.5 degrees C below ambient temperature, a net cooling power of 128 W.m(-2), a WCA of 161.2 degrees, and excellent anti-icing and self-cleaning performance. Finite-Difference Time-Domain (FDTD) simulations systematically reveal the regulation mechanism of the material's microstructure on light scattering efficiency. This work pioneers a novel approach for the high-value utilization of industrial by-products and provides an innovative solution for developing cost-effective, high-performance, and durable sustainable radiative cooling materials.
Aqueous ammonium-ion hybrid supercapacitors have attracted significant research interest due to advantages such as the abundant availability of NH4+, smaller hydrated ion radius, and faster diffusion rate. However, most NH4+ host materials suffer from limited capacitance. To address this challenge, this study introduces an interfacial engineering strategy that optimizes both the electrolyte composition and the active sites on the electrode surface through phosphate ion modification to facilitate H+ intercalation. By leveraging the co-intercalation of H+ and NH4+, a high capacitance of 1604.54 F g(-1) at a current density of 0.2 A g(-1) was achieved. In this system, ammonium sulfate is employed as the electrolyte to prevent MoO3 corrosion while supplying sufficient H+, whereas phosphate ions on the MoO3 surface act as effective intercalation channels for both H+ and NH4+. This study provides new insights into enhancing NH4+ storage capacitance in electrode materials through controlled
This study aims to overcome the limitations of traditional flame-retardant coatings, which suffer from inadequate multifunctionality, poor durability, and poor environmental friendliness. A two-step collaborative strategy of "porous structure construction + hydrophobic modification" was proposed. First, a three-dimensional interconnected porous flame-retardant coating was constructed by incorporating fibrous refractory fibers, flaky expanded graphite, and large-sized spherical hydrophobic silica (SiO2) particles into a waterborne epoxy resin matrix through morphological matching design. Subsequently, a room-temperature curable superhydrophobic slurry was developed using a polymethylhydrosiloxane (PMHS)-polydimethylsiloxane (PDMS)-hexadecyltrimethoxysilane (HDTMS) dynamic cross-linking system, synergistically combined with epoxy resin and multi-sized hydrophobic SiO2 nanoparticles. Finally, the slurry was sprayed to achieve gradient filling of the porous structure and low-surface-energy modification of the flame-retardant coating, resulting in a multifunctional composite coating integrating both flame retardancy and superhydrophobicity. Characterization results demonstrated a water contact angle (WCA) of 158 +/- 1.2 degrees and a sliding angle (WSA) as low as 3.5 +/- 0.8 degrees. After 6 days of water immersion, the water absorption rate decreased by 70 % and 58.6 % compared to the unmodified system and commercial products, respectively. Cone calorimetry tests revealed that the coated PVC substrate exhibited a 29.5 % reduction in peak heat release rate, a 64.7 % decrease in total smoke production, an 11.58-percentage-point increase in residual char yield, and a maximum smoke density temperature lowered to 81.7 degrees C, compared to the blank group. Under extreme conditions: the backside temperature of coated aluminum alloy plates stabilized at 218 degrees C (bare plates >500 degrees C) under 1100 degrees C butane flame impact, while coated wood maintained structural integrity after about 60 min of alcohol lamp burning (control group completely charred within 90 s). This work innovatively combines three-dimensional interconnected porous structures with hydrophobic modification, offering a novel strategy for developing high-performance and eco-friendly fireproof materials.
The potential of superhydrophobic coatings for anti-pollution flashover should be further explored, focusing on droplet electrical behavior on surfaces. In this study, the electrically driven behavior of droplets on a horizontal superhydrophobic surface was experimentally examined. The characteristics of this behavior were compared and analyzed relative to RTV (room temperature vulcanized silicone rubber). The findings indicate that droplets exhibit a propensity to undergo a rolling motion in the direction of the electric field on superhydrophobic surfaces. The electric field strength at the critical motion state of droplets on the superhydrophobic surface is observed to decrease with an increase in the water contact angle (WCA) of the surface. Moreover, it exhibits a distinct volume effect whereby the electric field strength initially decreases and then increases as the droplet's volume increases. The distribution of the electric field around droplets on a superhydrophobic surface was simulated, and volume effect analysis was conducted on the electric propulsion of the droplet. Electric propulsion of water droplets can remove pollutants along their path, enhancing anti-pollution capabilities on superhydrophobic surfaces in power systems.
MnO2-based electrode materials have attracted extensive research interest in aqueous ammonium-ion hybrid supercapacitors (A-HSCs) due to their low cost, environmental benignity, and high theoretical capacitance. However, their practical capacitance remains inferior to that of lithium-ion battery electrodes, largely due to the limitations of a pure NH4+ storage mechanism. In this work, Mo6+-doped MnO2 (MMN-2) was synthesized via a facile hydrothermal method. Experimental results demonstrate that Mo6+ doping promotes a H+/NH4+ cointercalation/deintercalation mechanism, substantially boosting the specific capacitance of MnO2. Moreover, Mo6+ doping optimizes the microstructure and pore size distribution of MnO2, improving electrolyte ion transport and structural stability during cycling. The MMN-2 electrode delivers a high specific capacitance of 586.2 F g- 1 at 2 mA cm- 2 and exhibits remarkable cycling stability, retaining 91.9% of its capacitance after 17,200 cycles. When assembled with activated carbon cloth (ACC) into an MMN-2//ACC A-HSC device, it achieves a maximum energy density of 0.787 mWh cm- 2 at a power density of 0.5 mW cm- 2. This work highlights Mo doping as an effective strategy to enable H+/NH4+ co-intercalation in MnO2, providing valuable guidance for designing high-performance ammonium-ion storage materials.
Adding short-chain methylammonium chloride (MACl) into the precursor solution of formamidine lead iodide (FAPbI3) is a commonly adopted strategy. This addition facilitates the generation of the alpha-phase and increases the grain size significantly. These changes in turn optimize the light absorption characteristics of perovskite thin films, thereby obtaining a high-quality perovskite thin film with uniform morphology and at the same time enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs). However, there are few reports of the use of longer alkylammonium chloride salts added to perovskite precursor solutions. Herein, we deliberately elected to introduce 2-fluoroethyl-1-amine hydrochloride (FEACl) into FAPbI3 as an alternative to MACl. The results indicate that FEACl can interact with perovskite precursors; this approach effectively enhances the crystallinity of perovskite thin films while promoting the stabilization of the alpha-FAPbI3 phase. Moreover, the large cations of FEACl are not incorporated into the lattice, which minimizes the change in the band gap of FAPbI3. The results show that PCE of the optimal device has increased from 23.07% of MACl treatment to 24.30% of FEACl treatment, and the filling factor (FF) has also increased from 81.95 to 84.37%, respectively. When unpackaged devices are stored at room temperature with a relative humidity ranging from 20 to 30% for 1000 h, the PCE is observed to be maintained at 83.57% of its initial value.
Constructing superhydrophobic surfaces has emerged as a promising anti-icing approach in recent years. However, the water droplets on the superhydrophobic surfaces are readily able to transition from the lowadhesion Cassie-Baxter (CB) state to the high-adhesion Wenzel state during the freezing process. Furthermore, the micro/nano structures of superhydrophobic surfaces are vulnerable to damage from mechanical loads. It remains a significant challenge to develop a robust superhydrophobic surface that can maintain the Cassie-Baxter state throughout the freezing and thawing processes. Herein, a micro-papilla/nano-particle (MPNP) structured superhydrophobic surface with good mechanical robustness and anti-icing property was prepared on aluminum substrate through laser ablation followed by spinning. The MPNP structure provides higher micro-features, denser nano-features, and a thicker hydrophobic layer, thereby endowing the surface with higher heat resistance, larger energy barrier, and Laplace pressure for water impaling in rough structures . Consequently, the MPNP surface exhibits excellent anti-icing property with a 6-fold prolongation in freezing delay time and a similar to 6-fold reduction in de-icing force in comparison to the bare Al substrate, and the droplet on this surface can maintain the CB state with mere 4.6 %/4.0 % decline in contact angle and 18.7 %/7.1 % increment in contact diameter in the freezing/thawing process. Moreover, owing to the protecting effect of the micro-papillae on the nano-particles, the thicker hydrophobic layer, and the interlock effect between the hydrophobic layer and rough structure, the MPNP surface can maintain super-hydrophobicity after a seize of mechanically robustness tests.
Both superhydrophobic bulk modification and coating have inherent limitations in providing waterproofing and anti-corrosion properties for concrete. This study developed a slurry with exceptional penetration at room temperature, seamlessly integrating superhydrophobic properties with concrete's inherent strength. After two applications of spraying, the slurry penetrates concrete blocks to a depth exceeding 10 mm. After 2 min of spraying the slurry at room temperature, the concrete exhibits hydrophobic properties, achieving super- hydrophobicity after 7-9 h, with a water contact angle of 156 +/- 0.5 degrees and a sliding angle of 3 +/- 0.5 degrees. Treated concrete blocks show at least a 70 % reduction in water absorption after immersion in various solutions for 30 days. They also demonstrate strong resistance to freeze-thaw cycles, temperature shocks, electrochemical corrosion, abrasion, and UV radiation. This innovative method offers a promising approach for designing superhydrophobic concrete, thereby enhancing its practical applications in engineering.
Icing can cause huge inconveniences in daily life and even safety problems. Constructing photothermal superhydrophobic coatings is considered as a promising strategy for inhibiting ice accretion due to their good passive anti-icing and active de-icing capability. However, such coatings usually involve high-cost photothermal materials, toxic fluorinated reagents, fragile nanostructures, and inferior chemical stability. This study proposes a novel strategy for fabricating a triple-scale photothermal superhydrophobic coating (TPSC) through a simple impregnation method using inexpensive green petroleum coke (GPC) particles (submillimeter scale) and nanoscale graphite (Gr) particles. The TPSC is superhydrophobic with a water contact angle of 160.3° and possesses an excellent photothermal property with a temperature increase of ∼42 °C under 80 mW/cm2 irradiation with sunlight. Owing to its superhydrophobicity, the freezing time of the TPSC is prolonged by a factor of 7.87 compared with that of bare aluminum. Benefiting from the excellent photothermal effect, an ice droplet on the coating can be melted within 180 s under 60 mW/cm2 irradiation with simulated sunlight. Furthermore, the incorporation of GPC not only effectively protects the embedded Gr particles within the microgrooves but also stabilizes the Cassie-Baxter state, thereby significantly enhancing the mechanical robustness and chemical stability of the TPSC. More importantly, this approach avoids the carbon emissions associated with the calcination of GPC, achieving an environmentally friendly and cost-effective application. This study can be expected to offer an efficient and sustainable anti-icing and de-icing strategy for outdoor equipment.
The imperative to address global water scarcity has intensified the pursuit of atmospheric water harvesting (AWH) technologies. However, achieving ultraefficient AWH remains a formidable challenge. Herein, a pioneering porous COFs@PVDF (PCP) film, exhibiting a water contact angle of 157.5 degrees and a low sliding angle of 4 degrees, has been engineered for ultraefficient AWH from fog. Notably, the integration of superhydrophilic covalent organic frameworks (COFs) within the poly(vinylidene fluoride) (PVDF) matrix represents a strategic innovation, resulting in an ultrahigh water collection rate of 3.080 gcm-2h-1 during fog-based AWH by polymer composites. Compared to the porous PVDF film, the PCP's water collection rate has witnessed a staggering increase of 286%. Significantly, this marks the successful instance of COFs being reported in fog-based AWH. Density functional theory calculations reveal that the adsorption energy for H2O has escalated from -0.28 to -0.44 eV due to the integration of COFs, underscoring the pivotal role of COFs in enhancing the AWH performance. Moreover, the PCP film's self-cleaning capabilities, mechanical robustness, and chemical stability highlight the film's potential application for large-scale deployment in AWH. This work presents a groundbreaking approach to fog-based AWH, significantly contributing to global water security and addressing critical water scarcity issues.
The electrocatalytic urea oxidation reaction (UOR) is a promising approach to lowering the energy barrier of the anode half-reaction in water splitting for energy-efficient hydrogen production and to remove excess urea from blood or dialysis fluid. However, the sluggish kinetics and large overpotential caused by scaling relationships significantly limit the development of the UOR technology. Herein, bifunctional amorphous M-CoS (M = Zr, Cu, Mn, Fe) nanosheets were synthesized via a one-step electrodeposition process. Among them, Zr-CoS exhibited exceptional electrocatalytic performance, achieving 10 mA cm-2 in UOR at an overpotential of 1.26 V, outperforming recently reported catalysts, while CoS demonstrated 10 mA cm-2 in the hydrogen evolution reaction at an impressively low overpotential of -175 mV. Density functional theory calculations revealed that doped Cu and Zr ions migrated to the adsorption sites of N atoms before and after C-N cleavage, breaking the limitation of scaling relationships. Meanwhile, the energy barrier of the C-N cleavage step showed a good linear relationship with the variation of integrated crystal orbital Hamilton population (ΔICOHP), indicating that ΔICOHP was a good descriptor to evaluate UOR performances. This work not only emphasized the outstanding performances of Zr-CoS but also offered innovative insights into the role of metal sulfides in UOR.
VOx, possessing multiple stable oxidation states, demonstrates high theoretical capacity, rendering it a promising candidate for supercapacitor electrodes. However, its practical capacity and cyclic performance are hindered by low electrical conductivity and sluggish diffusion kinetics. Incorporating heteroatoms into transition metal oxides has emerged as an effective approach to mitigate these challenges. Nonetheless, the reported capacities and cyclic stabilities of single-element-doped-VOx as supercapacitor electrodes remain unsatisfactory. Herein, we propose a Co/Cu/C multi-doped VOx composite (VCoCuC) nanobelts, which significantly boosts the specific capacity (5.96 C cm(-2)/3 98.6 C g(-1) @ 10 mA cm(-2)) and cycling performance (97.1% of the initial capacity after 2,000 cycles @ 60 mA cm(-2)) compared to samples with only Co/Cu, Co/C, or Cu/C doping. The possible functions of each doping element are discussed. Additionally, an aqueous asymmetric supercapacitor with VCoCuC as the cathode and conductive carbon cloth (CC) as the anode is assembled to demonstrate the potential application of VCoCuC, which delivers high energy density and excellent cyclic performance. These findings highlight the potential for improving the practical capacity and cyclic performance of VOx electrodes via a multi- doping strategy.
Repairable superhydrophobic surfaces have promising application potential in many fields. However, so far, it is still a challenge to develop a superhydrophobic surface with repairability for multiple types of damage through a simple method. In this paper, a repairable superhydrophobic coating was obtained on various substrates by blade-coating mixtures of polydimethylsiloxane (PDMS), polyvinylidene fluoride (PVDF), and multiwalled carbon nanotubes (MWCNTs) modified with dopamine (PDA) and octadecylamine (ODA). The obtained coating has a good liquid-repellent property with a water contact angle above 150° and a water sliding angle of ∼6° and possesses an excellent absorbance (∼97%) in the wavelength range of 250-2500 nm. Due to its high absorbance, the coating displays an outstanding photothermal effect with a temperature rise of ∼65 °C under irradiation by 1.0 kW/m2 of simulated sunlight. Furthermore, after being degraded by multiple stimuli, including plasma treatment, acid/alkali/oil immersion, sand impact, and the icing-thawing cycle, the coating can recover superhydrophobicity via sunlight irradiation, demonstrating the good photothermal-induced repairability of the coating. It can be expected that the good water-repellent property, photothermal effect, and repairability give this coating a promising prospect in practical applications.
Perovskite solar cells (PSCs) are celebrated for their potential in clean and renewable energy applications. However, their performance and longevity are often compromised by surface and grain boundary defects. Herein, a posttreatment strategy using 4-hydroxy-4 '-biphenylcarboxylic acid ethyl ester (EHBC) is introduced to passivate these defects in perovskite films, thereby enhancing the performance of PSCs. As a Lewis base, the carbonyl group of EHBC interacts with uncoordinated lead ions to passivate lead vacancy defects, while the hydroxyl group forms hydrogen bonds with iodide ions, reducing their migration. Additionally, the hydrophobic biphenyl groups of EHBC enhance the resistance to moisture. The study demonstrates that PSCs treated with EHBC retain 69% of their initial performance after 700 h under 30% relative humidity, achieving a maximum power conversion efficiency (PCE) of 24.48%, a significant improvement over the untreated control PSCs (PCE = 23.04%). This synergistic passivation strategy offers an effective approach for fabricating high-efficiency and stable PSCs.