In pursuit of greener and more sustainable textile dyeing processes, this study employed laccase (Lac) to catalyze the polymerization of vanillic acid (VA) for cotton dyeing. Cotton fabric was first aminated with 2-chloro-4,6-diamino-1,3, 5-triazine (CDATA), and VA was subsequently polymerized on the modified fabric under the catalysis of Lac to achieve dyeing. The structure of polyvanillic acid (pVA) obtained via enzymatic polymerization and its polymerization mechanism were elucidated using UV-Vis spectroscopy, FTIR, and UHPLC/ESI/MS. Fabric dyeing performance was evaluated via K/S measurements and color fastness. The surface elemental composition and amino-group content of the modified cotton were determined by XPS and a PNBD-based UV–Vis method. Molecular simulations were used to examine representative interaction configurations among pVA, CDATA, and cellulose. Notably, this work demonstrates a Lac-mediated enzymatic polymerization strategy enabling simultaneous coloration and multifunctional finishing of cotton fabrics via in situ formation and immobilization of pVA on aminated cotton. The results showed that VA mainly formed colored pVA products through phenoxy (Ph–O) and phenyl–phenyl (Ph–Ph) linkages under Lac catalysis. Under the optimized conditions, the amino-group content of the modified cotton reached 2.252 × 10−3 mmol g−1, the K/S value of the dyed fabric was 2.53, and most color-fastness grades improved by 0.5–1 grade after CDATA modification. The dyed fabric exhibited a UV protection factor (UPF) of 71.43, inhibition rates of 96.95% against E. coli and 99.99% against S. aureus, and a DPPH radical-scavenging rate of 77.96%, together with enhanced thermal stability and mechanical properties. This study integrates biocatalysis with fabric surface modification, providing an eco-friendly approach for multifunctional textile finishing.
Inspired by the layered structure and mechanical robustness of jellyfish mesoglea, this study uses lignin extracted from waste Apocynum venetum L. stems by deep eutectic solvent extraction to construct an anisotropic hydrogel with ordered layered pores. Flexible polyvinyl alcohol chains form a reversible covalent cross-linked network with lignin through dynamic imine bonds. The incorporation of MXene nanosheets, which feature multi-level hydrogen-bonding, further endows the hydrogel with photothermal conversion capabilities. The lignin-based hydrogel combined high compressive strength of 6.81 MPa with an ultrahigh water content of 91.6 wt%, and retained 82.4% of its initial stress after 100 compression cycles. The hydrogel also exhibited a breaking stress of 9.70 kPa and a breaking strain of 755%, indicating good tensile deformability. Owing to the oriented pore structure and regulated hydration environment, the hydrogel delivered solar-driven interfacial evaporation with an evaporation rate of 2.88 kg m−2 h−1 and an efficiency of 95.8% under 1.0 sun irradiation. The hydrogel also showed broad-spectrum antibacterial activity, with inhibition rates of 99.99% against E. coli and S. aureus. These results demonstrate that coupling a dynamic hydrogen-bond network with a biomimetic architecture is an effective route to biomass-derived hydrogel evaporators with high water content and high evaporation efficiency.
Precise sieving of structurally similar solutes in organic solvents is crucial for chemical industries such as pharmaceutical synthesis and petroleum refining. However, it remains technically challenging due to their similar physicochemical properties. Achieving this with organic solvent nanofiltration (OSN) requires membranes with narrow pore-size distribution and tailored surface chemistry. Herein, we report an additive-free strategy to prepare ultrathin, structurally homogeneous polyamide (PA) nanofilms via alkyl chain engineering during interfacial polymerization (IP). Alkyl chains synergistically regulate the diffusion kinetics and the reaction process: they enable rapid, uniform amine supply while introducing steric hindrance that moderates polycondensation. This dual regulation yields a structurally homogeneous PA layer with sub-nanometer pores. The optimized membrane shows a sharp rejection curve and effectively separates antibiotics, demonstrating promise for pharmaceutical purification. This work advances the understanding of diffusion-reaction synergy in IP and offers a facile strategy for precision separation membranes.
Electrocatalytic CO2 reduction (ECO2RR) is a promising route to sustainable fuel and chemical production, yet its practical application is hindered by the formidable challenge of precisely controlling product selectivity. In recent years, electrolyte engineering, particularly the regulatory role of halide ions, has attracted considerable interest due to their significant influence on the catalyst's surface/interfacial microenvironment and reaction pathways. This review focuses on halide ions as a key tool, systematically elaborating on how they induce dynamic surface reconstruction and specific crystal facet exposure in catalysts through specific adsorption, tune surface roughness to increase active site density, modulate the catalyst's electronic structure via their unique electronegativity to stabilize key active valence states, optimize the adsorption behavior of critical reaction intermediates, and thereby steer reaction pathways. The synergistic mechanism of dynamic surface reconstruction-valence stabilization-electronic structure tuning-pathway guidance is summarized to provide insights for the rational design of efficient and highly selective ECO2RR catalysts.
In order to promote the sunlight utilization ability of wood based photocatalyst, a facile in-situ synthesis strategy was employed to fix cuprous oxide (Cu2O) and multi-walled carbon nanotubes (MWCNTs) on wood substrate. The resulting MWCNTs/Cu₂O@wood composite could photocatalytically degrade 97.91% of methylene blue (MB) within 9 h and maintain over 95% efficiency after 50 cycles, and the desirable degradation capability toward malachite green and crystal violet was obtained as well. Furthermore, 95.6% of formaldehyde and 96.9% of acetone in air could also be removed within 12 h under visible light irradiation by the modified wood. It's the first time that the unique cage-like structure of MWCNTs was successfully fabricated on wood surface in this work, which effectively trapped visible light, enhanced light utilization and finally promoted the photoresponse capability of the modified wood. Simultaneously, the cage-like configuration facilitates the enrichment of organic pollutant molecules, increasing the contact area between the photocatalyst and pollutants and thereby improving the overall photocatalytic performance. The in-situ synthesized MWCNTs/Cu2O on wood substrate in this work proposed a potential approach to develop efficient and durable wood-based photocatalysts, suitable for air and water purification.
Solar-driven interfacial desalination is attractive for decentralized freshwater production, yet practical evaporators still face challenges associated with intermittent water supply, insufficient heat localization, and structural degradation during operation. Herein, a MOF integrated Janus cellulose aerogel (denoted as PAC@MOF-CB) was designed as a moisture-assisted solar desalination platform. The aerogel combines a hydrophilic moisture-harvesting layer containing amino-functionalized MOF-801 with a carbon black (CB) based photothermal evaporation layer. The MOF-containing layer provides Zr-OH, amino, and microporous adsorption sites for water uptake, whereas the CB layer concentrates solar energy at the evaporation interface. This Janus configuration spatially couples atmospheric moisture storage, water transport, and solar-driven vapor generation in an elastic porous framework. PAC@MOF-CB exhibited a water uptake of 0.511 g·g−1 at 30% RH and reached 68.8 °C within 90 s under 1 sun irradiation. The evaporation rate reached 2.25 kg·m−2·h−1 under simulated sunlight. For real Yellow Sea seawater and Sayram Lake water, the condensate showed more than 99.9% rejection of the measured major cations, including Na+, K+, Ca2+, and Mg2+. This study demonstrates a Janus aerogel design for coupling moisture harvesting with solar interfacial desalination, offering a feasible material strategy for freshwater generation in water scarce environments.
Membrane separations without phase transition offer a compelling route to low-energy crude oil fractionation. For practical implementation, membranes are required to simultaneously achieve high permeance, sharp molecular sieving and long-term structural stability in hydrocarbon media. Herein, we report the rational design of homogeneous polyamide membranes for crude oil separation, fabricated via oil-soluble surfactant mediated interfacial polymerization by synergistic integration of hydrophobic monomers. The rigid fluorinated monomer improves membrane compatibility with hydrocarbons, while oil-soluble surfactants with varying chain lengths enable the regulation of pore size distribution, yielding a wrinkled and ultrathin selective layer. The modulated membrane exhibits precise sieving of small solutes, showing a high toluene/triisopropylbenzene separation factor of ∼14 and excellent permeance of ∼8.4 L m-2 h-1 bar-1. Importantly, the membrane retains superior selectivity for light crude oil separation, enabling effective retention of heavy components and delivering a light permeate with lower boiling point distribution. This work advances the development of sustainable membrane technologies for efficient crude oil separation.
Solar-driven interfacial evaporation is a promising strategy for desalination and wastewater purification, but many efficient evaporators still rely on synthetic photothermal materials that are costly and may pose environmental risks. Herein, a biomass evaporator without photothermal filler doping was developed by integrating spent-coffee-grounds derived nanocellulose with soy sauce based melanoidin-rich components. The abundant amino-containing compounds within these biomass-derived components enabled Schiff-base crosslinking with aldehyde-functionalized nanocellulose, thereby immobilizing the photothermal components within the nanocellulose network. The resulting composite was further reinforced by polyvinyl alcohol, Ca2+-mediated crosslinking of sodium alginate, and hydrogen-bonding interactions, generating a multilevel crosslinked polymer network. After freeze-drying, a porous aerogel was obtained and denoted as CGF@SS aerogel. Inspired by the cap-stipe architecture of mushrooms, the CGF@SS aerogel was integrated with a cotton wick functioning as both a water-transport pathway and a thermal insulation support, thereby forming a biomimetic mushroom-shaped evaporator designated as the MS-CGF@SS evaporator. This architecture enabled continuous water supply, interfacial heat localization, and reduced conductive heat loss to bulk water. Benefiting from broadband light absorption by soy sauce-derived melanoidin-rich components and biomimetic heat and water management, the evaporator achieved an evaporation rate of 2.996 kg m−2 h−1 and a solar-to-vapor conversion efficiency of 89.3% under 1.0 sun, while maintaining an outdoor average evaporation rate of 2.50 kg m−2 h−1. When treating seawater and dyeing wastewater, the condensate met drinking-water ion limits, while the purification process enabled effective dye rejection and significant reductions in chemical oxygen demand, ammonia nitrogen, suspended solids, and total phosphorus. This work offers a sustainable route for converting food and agricultural wastes into environmentally compatible solar evaporators.
Halide ions dynamically engineer the catalytic interface across multiple dimensions, directing ECO 2 RR selectivity.
Epoxy resin (E-51) exhibits excellent adhesion and is widely used in the preparation of functional composite coatings. However, its smooth surface lacking micro/nano composite structures limits its self-cleaning capability and optical properties. Direct incorporation of organic silicone or inorganic fillers often faces severe phase separation and filler agglomeration issues, resulting in defects in coating durability and weather resistance. To address these challenges, this study developed a synergistic modification strategy integrating surface energy modulation with the architectural design of micro/nano-structures. Amino-terminated PDMS undergoes ring-opening addition reactions with epoxy groups in the epoxy resin, while functionalized barium sulfate nanoparticles modified with dual silane coupling agents are incorporated to enhance optical properties. This synergistic approach not only resolved interfacial compatibility but also endowed the PDMS@EP-BaSO4 coating with outstanding comprehensive properties; the water contact angle increased to 123.5°, demonstrating an easy-to-clean benefit. Visible light reflectance reached 95%, and emissivity rose to 90%. Furthermore, when applied to metal surfaces, the coating exhibited excellent stability against acid-alkali-salt corrosion, extreme temperatures, and ultrasonic agitation. This work provided a novel approach for developing protective coatings that integrated high reflectance, high emissivity, and long-term anti-soiling properties.
Single-atom alloy (SAA), consisting of foreign atoms diluted within the matrix of a host metal, represents a captivating atomic ensemble that balances affordability and activity. Their catalytic performance is largely governed by the synergistic interactions between the doped metal atoms and the host metal. However, how such synergy correlates with the structural characteristics of the two metal sites—including the aggregation state of the doped single atoms and the oxidation state of the host metal—remains insufficiently understood. Here we use well-defined PdCo SAA model catalysts for electrochemical nitrate reduction to ammonia to quantify the relationship between metal-site synergy and these structural descriptors. Specifically, increasing the degree of Co single-atom aggregation promotes NO3⁻ chemisorption and enables the reaction to circumvent the energetically demanding NH3 desorption step associated with the NOH pathway. However, excessive Co aggregation induces overly strong binding of reaction intermediates, which can be mitigated by increasing the oxidation state of the Pd substrate and thereby raising its work function. As a proof of concept, the Co20/PdO catalyst delivers Faradaic efficiencies exceeding 96% across a broad pH range. When implemented in a membrane electrode assembly, it further achieves 1000mAcm–2 at 2.30V and sustains stable operation for 850h at 500mAcm–2, while maintaining NH3 selectivity above 90% and an NH3 production rate of 2.09mmolh–1 cm–2.
To develop a green enzymatic method for the remediation of parabens (PBs) contaminants, a ternary composite system comprising laccase, 2, 2, 6, 6-tetramethylpiperidine-1-oxyl (TEMPO) mediator, and cutinase SE50 (LCTM) was constructed. Using methylparaben (MP) as a model substrate, the degradation performance, kinetic characteristics, and underlying mechanisms of the system were systematically investigated. The results demonstrated that TEMPO significantly enhanced the catalytic conversion of MP by laccase, and the subsequent introduction of cutinase SE50 further boosted the overall degradation efficiency. Under the optimized conditions (0.5 U/mL cutinase SE50, 1.2 U/mL laccase, 25 mg/L TEMPO, temperature 50 °C, and pH 6.0), the degradation rate of MP reached 96.8
Chiral separation membranes have demonstrated their significant potential for the efficient separation of racemic mixtures into enantiopure components. However, the preparation of membranes with both high enantioselectivity and flux remains a challenge. Herein, we adopted the free-interface interfacial polymerization strategy for fabricating ultrathin chiral amino-beta-cyclodextrin (CCD) membranes. By applying solvent-activated amino beta-cyclodextrin with superior chirality as the only reagent in aqueous phase, we successfully fabricated defect-free CCD enantioseparation membrane with sufficient chiral sites, exhibiting remarkable performance in separating racemic DL-phenylalanine, achieving an enantiomeric excess (ee %) value of 96.64 % and a flux of 1.01 mmol center dot m- 2 center dot h- 1. The unexpected performance of the CCD membrane is realized following a process of CD activation within dimethylformamide (DMF), during which the interaction with the solvent generates the appropriate structure changes. These changes enhance a binding energy difference between activated amino-beta-CD and enantiomers (D/L-phenylalanine) that is absent in the non-activated one, attributed to a differential hydrogenbond interaction state. The findings underscored the potential of integrating the chiral selectivity of cyclodextrin with the ultrathin properties of nanofilm to create efficient chiral separation membranes, thereby advancing the development of high-performance cyclodextrin-based materials for chiral separation.
Photoelectrochemical syngas production using photoanode-driven systems from aqueous CO2 is a promising technology. To address the challenge of poor selectivity caused by the wide band gap of photoelectrode, we introduce a novel photoanode, PDI/Cu2O/Cu, where PDI is the perylene tetracarboxylic di-(propyl imidazole). Using Cu2O as a substrate enhances charge transfer kinetics, while PDI modification mitigates photocorrosion and augments photoelectrochemical CO2 reduction reaction (PEC CO2RR) activity. This enhancement stems from PDI’s narrow band gap and efficient visible light absorption. The syngas production achieved a noteworthy 124.47 μmol/(cm2·h) at 1.57 V vs. RHE, making it an optimal feedstock gas for hydrocarbon synthesis. Detailed UV–vis spectra indicate that layered structure significantly improves the absorption edge of the photoanode, facilitating enhanced utilization of visible light. Additionally, the electron lifetime of the PDI/Cu2O/Cu photoanode is substantially increased which is also one of the factors affecting the reactivity, as demonstrated by the Bode phase plot.
Extending carbon dioxide (CO2) electrocatalysis to afford energy-rich carbohydrates with long carbon chains is significant but still suffers from unsatisfactory selectivity for products with more than three carbon atoms. Here, using CO2 as the only carbon feedstock, we present a cascade electrolysis strategy for succinic acid (SA; C4H6O4) synthesis by coupling CO2 electroreduction with electrocarboxylation of in situ-generated ethylene (C2H4). An overall CO2-to-C4H6O4 conversion was achieved. Our findings illustrate that adsorption of in situ-generated C2H4 and the rate-determining step (*C2H4 to *C2H4COO) occur more easily over FeNi foam. Notably, compared with typical CO2 reduction products, converting gaseous CO2 into SA lowers separation costs, enhancing economic viability. Our strategy also significantly reduces carbon emissions (-0.174 kg CO2 per kg SA), compared with conventional strategies (1.94 for petrochemical and 0.88 for bio-based SA). This system accelerates CO2 conversion into long-chain carbohydrates, facilitating reintegration of this industrial waste gas into the global economy.
The development of electro-thermal textiles has attracted growing interest as a promising approach for active thermal management in wearable systems. Metallic-coated fabrics can efficiently generate heat through the Joule effect; however, their long-term performance and safety are severely limited under perspiration due to metal ion release and corrosion. To overcome these challenges, this study introduces a Parylene-C encapsulation strategy for copper-coated polyethylene terephthalate nonwovens (CuPET) using a chemical vapor deposition (CVD) process. The conformal, biocompatible Parylene-C films (thickness 4–16 μm) act as effective protective barriers while preserving the porous textile structure. Morphological and comfort analyses demonstrate a controlled reduction in air permeability from 3100 to 1100 L·m−2·s−1, maintaining acceptable breathability. Electro-thermal measurements reveal rapid and uniform heating, reaching 40–45 °C within 2 min at 2 V, and the addition of a thermal insulation layer further enhances the Joule heating efficiency, increasing the steady-state temperature by approximately 6 °C. ICP–OES results show an ≈80% reduction in copper ion release (from 28.34 mg·L−1 to 5.80 mg·L−1) after artificial sweat exposure. This work demonstrates a scalable encapsulation route that effectively balances sweat protection, electrical stability, and thermal performance, paving the way for safe, durable, and actively heated smart textiles for advanced thermal insulation applications.
Although the application of solar-driven interfacial evaporation technology in the field of seawater desalination has seen rapid progress in recent years, mediocre water evaporation rates remain a longstanding bottleneck. The key to resolving this bottleneck is leveraging strong hydrogen bonding to reduce the enthalpy of evaporation for water molecules and inputting environmental energy. This study presents a novel approach for reducing the enthalpy of vaporization by introducing a hydrophilic inorganic material Al(H2PO4)3 (AP) on the surface of cellulose nanofibers (CNF) to form an inorganic‒organic hydrogen-bonded network in cellulose-based hydrogels (labeled 3DL Metagel). This network structure accelerates the diffusion of water molecules between CNF, as confirmed by molecular dynamics simulations. Specifically, inspired by multiple biological traits found in nature, the 3DL Metagel evaporator integrates a lotus shape, Janus wettability (the superhydrophilic lotus-like flower with hydrophobic lotus-like leaves) and plant transpiration, resulting in superior water evaporation rates of up to 3.61 kg·m−2·h−1 under 1.0 solar radiation (exceeding the limit of two-dimensional evaporators). The unique lotus shape enables 3DL Metagel to draw additional energy from the environment during desalination, resulting in a maximum water evaporation efficiency of 94.94