ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Wang Zhao,Cheng Xu,Nuo Xu,Guitao Du,Xiangli Gao,Jianbo Shuai,Zepeng Lei,Xiaohui Wang
With the increasing global demand for sustainable polymers, scalable routes that convert cellulosic feedstocks into high-performance materials are urgently needed. However, efficient dissolution and regeneration of cellulose (CEL) without sacrificing its native degree of polymerization (DP) remain a central challenge in the processing of cellulosic materials. Here, we introduce a hydrophobic-engineered amphiphilic ionic-liquids (AILs) platform that meets this goal. A homologous series of AILs was synthesized by grafting n-alkyl chains of tunable length onto a superbase cation. The resulting AILs dissolve CEL up to 5 times faster than state-of-the-art imidazolium ionic liquids while preserving DP values close to those of the native polymer. Long-time scale (300 ns) molecular-dynamics simulations reveal that the hydrophobic tail of the cation blankets glycosidic linkages against chain scission, whereas the ionic component disrupts inter- and intrachain hydrogen bonds to promote dissolution. This gentle and efficient processing method lowers energy demand and chemical waste, thereby reducing the environmental footprint of biobased material production. By leveraging designable, recyclable AILs, it adheres to green-chemistry principles and supports a circular materials economy. These findings reveal that the amphiphilicity tuning of ionic liquids could be applied as a practical design principle for gentle and efficient processing of sustainable biobased materials.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Changqing Yuan,Haohao Wei,Xiaorong Meng,Han Shen
Vanadium oxides are regarded as one of the most promising cathode materials for aqueous zinc-ion batteries (AZIB). Among them, vanadium dioxide (VO2) has garnered significant attention due to its unique tunnel structure and superior electrochemical performance. However, VO2 also exhibits certain limitations, such as insufficient stability and poor tolerance to high currents. To enhance the rate capability of VO2, a mixed-valence form of VO2 with improved rate performance was synthesized by adjusting the amount of the reducing agent (i.e., H2C2O4·2H2O). Subsequently, a VO2/g-C3N4 composite material was fabricated using an in situ growth method. Research findings indicate that the rate capability and stability of VO2 are markedly enhanced upon combination with g-C3N4. This improvement is attributed to the protective effect of g-C3N4 on VO2. Moreover, the g-C3N4 synthesized via the solid-state method features a porous structure, which facilitates the normal intercalation and deintercalation of Zn2+ ions, providing numerous pathways for Zn2+ movement. Additionally, EDS-mapping images reveal that nitrogen (N) elements from g-C3N4 are successfully doped into VO2 nanorods. The incorporation of N elements significantly boosts the conductivity and ionic diffusion of the composite. The resulting material achieves an exceptionally high specific capacity of 500.18 mAh/g at the current density of 0.2 A/g, and it maintains a specific capacity of 282.54 mAh/g even at a high current density of 10 A/g. After 10,000 charge–discharge cycles, the capacity retention rate remains as high as 87.33% at 10 A/g, demonstrating a substantial improvement in both rate capability and cycling stability. This study provides compelling evidence for the application of mixed-valence vanadium oxides as cathode materials for AZIB and offers valuable insights into the development of vanadium oxide composite materials.
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Hui Hu,Honghui Xie,Sanqi Liang,Mengting Yu,Fanglin Liu,Shengjun Deng,Shuhua Wang,Weiming Xiao,Chao Chen
The reports on MOFs supported nonprecious metal nanocatalysts (NPM/MOFs) remain limited, primarily due to the conflict between the harsh conditions for the preparation of nonprecious metal nanoparticles and the poor stability of MOFs; the fabrication of NPM/MOFs has long been a challenge. Herein, we demonstrate a facile, versatile, and sustainable method to fabricate NPM/MOFs by directly reacting commercial metal dusts with the ligands through simple ball milling. In this approach, the metal dusts were sacrificed in situ to form the corresponding MOFs and etched into smaller nanoparticles at the same time. The developed approach entirely circumvents the harsh conditions typically required for the preparation of nonprecious metal nanoparticles, while preserving the porous structures of the MOFs. By this facile approach, several NPM/MOFs with intact pore structures were prepared. Moreover, this approach consumes trace amounts of solvent, conforming to the concept of sustainable synthesis. In addition, the synthesized Co/ZIF-67 nanocatalyst was tested in the hydrogenation of unsaturated aldehydes; it exhibits an exceptionally catalytic performance that is comparable to many noble metal nanocatalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2025
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IF 11.3
Jinhua Liu,Huaijun Xie,Jianjiang Lu,Qing Xie,Jingwen Chen
Indoor semi-volatile organic compounds (SVOCs) pose significant health risks due to their widespread presence. However, their comprehensive profiling remains difficult due to the inherent limitations of conventional active sampling techniques and targeted analytical approaches. Here, we present an integrated approach that combines polydimethylsiloxane (PDMS) foam-based passive air sampling with non-targeted analysis for high-throughput screening and semi-quantitative evaluation of indoor SVOCs. Two passive samplers, specifically optimized for capturing gas-phase and particle-bound SVOCs, were calibrated under real-world indoor conditions. The experimentally derived sampling rates were then used to construct predictive models aimed at extending quantitative applicability across diverse compounds. In addition, a reference-compound-based semi-quantitative strategy was established to support the non-targeted analysis. Field application in a building material market showed strong agreement between passive and active sampling results for both gas-phase and particle-associated SVOCs. Overall, this integrated approach enhances conventional indoor air monitoring by enabling broader chemical coverage and semi-quantitative analysis, offering a practical tool for exposure assessment and risk-informed chemical management.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Jing Wang,Zhixuan Ma,Shuai Wang,Shufeng Shen
Recent advancements have positioned nonaqueous amine-based absorbents as promising candidates for energy-efficient CO2 capture. However, detailed physicochemical data are still essential to support accurate modeling for scaling up the process. Diffusivity (D) and physical solubility (H) of N2O and CO2 in organic solvents were determined by using a stirred cell. Gas solubility ratios (HCO2/HN2O) in these solvents exhibit an inverse correlation with the solvents’ Hoy solubility parameters. Changes in the DCO2/DN2O ratio and D^(1/2)/H in various solvents are governed by interactions between gas properties and solvent polarity. Specifically in the 2-hexyloxyethanol (2-HE)/2-(ethylamino)ethanol system, DN2O was found to be inversely proportional to solvent viscosity with a power of 0.6. The ratios of the derived combined parameter D^(1/2)/H for CO2 and N2O increase with solvent polarity. This correlation framework allows reliable prediction of transport properties in the 2-HE based nonaqueous system, supporting kinetic study and scalable carbon capture design.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yingying Li,Guangyao Zhang,Deqi Fan,Zongze Li,Yi Lu
Achieving efficient and selective solar-driven CO2 reduction remains a grand challenge due to sluggish proton–electron transfer kinetics and limited reactant availability at catalytic interfaces. Herein, we present a hierarchically structured aerogel integrating triazine-based covalent organic frameworks (TCOF) with Nb2CTx MXene nanosheets embedded in a poly(vinyl alcohol)/sodium alginate (PVA/SA) matrix. The aerogel leverages broadband light harvesting, hierarchical water regulation, and localized photothermal activation to enhance multielectron CO2 conversion. The hydrophilic–hydrophobic PVA/SA scaffold promotes rapid water uptake and vapor-phase transport, while Nb2CTx enables efficient near-infrared-induced heating to establish a proton-rich interfacial microenvironment. Simultaneously, the porous TCOF network offers abundant CO2 adsorption and activation sites. This synergistic architecture facilitates stable proton-coupled electron transfer (PCET) pathways and C–C coupling. In situ spectroscopic analyses reveal enhanced formation and stabilization of *COOH, *CH3, and *OCCHO intermediates under photothermal conditions, evidencing facilitated C–C coupling for C2 product generation. Under 3-sun irradiation for 3 h, the optimized TCOF/Nb2CTx aerogel delivers exceptional yields of 119.3 μmol·g–1 CH4 and 94.9 μmol·g–1 C2H4, which is 2-fold higher than powder analogues and surpassing previous COF/MXene systems. This work demonstrates a generalizable strategy to engineer carbohydrate polymer-based aerogels with integrated light-to-heat conversion, vapor regulation, and catalytic site accessibility for efficient solar-to-chemical fuel generation.
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ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Xueqin Du,Qiuhong Li,Zhenhe Wang,Hao Liu,Guangxian Wang,Wei Chen,Mario Caironi
Fluorescent sensors are promising for efficient and pervasive healthcare and environmental monitoring. Such wide research interest has not yet delivered practical applications owing to a series of limitations of adopted fluorescent molecular probes. One of the key limitations is the versatility of such probes, typically not active on a wide pH spectrum or not sensitive to multiple stimuli. In this study, we demonstrate dual fluorescence response of a tetrastyrene (TPE) derivate, namely ((1E)-((4- (1,2, 2-triphenylvinyl-benzylidene)hydrazine)methyl)ferrocene (Fc-TPE), which shows responses to both acidic and alkaline environments. This phenomenon is possible due to hydrolysis of imine bonds under both acidic and alkaline conditions, which hinders competitive photoinduced electron transfer, thus enabling dual pH dependent fluorescent emission. At the same time, the sensitivity of the imine bonds to some cations can be exploited to trigger the same fluorescent switch for the detection of elements that present a health hazard for humans. As proof-of-principles of the multiresponsive capabilities, we report an Fc-TPE based hydrogel obtained by simple one-pot synthesis exhibiting a reversible fluorescent switching, allowing to monitor fish and meat freshness, as well as Cu2+ detection in solution. Our results can have a significant impact in delivering fluorescent molecular probes to smart optical sensors with relevant practical applications.
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ACS Biomaterials Science & Engineering
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2025
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IF 5.5
Bo Li,Chenchen Li,Ziyi Yan,Ping Ji,Xiaoling Yang,Hongsi Yu,Congyan Xia,Fengyi Xie,Meilin Zhao,Bo Hu
Promoting the regeneration of bacteria-infected damaged tissues by developing multifunctional tough hydrogels with self-healing, adhesive, remodeling, and antimicrobial properties for use as wound dressings remains a great challenge. Inspired by the excellent adhesion ability of natural mussels, hyaluronic acid (HA) was first oxidized to aldehyde hyaluronic acid (AHA), and then grafted with dopamine (DA) to produce a structure with many catechol groups from which dopamine-grafted hyaluronic acid (DAHA) was prepared and combined with acrylamide (AM), poly(acrylic acid) (PAA), and N,N′-methylenebis(acrylamide) (BIS) to prepare a multifunctional hydrogel (PAD hydrogel). The results indicated that the PAD3 hydrogel with a DAHA content of 3 mg/mL and a BIS monomer content of 0.5 mol %, had high mechanical strength (over 10 MPa), which was 27 times greater than that of pure polyacrylamide (PAM) hydrogels. Furthermore, the PAD hydrogel demonstrated strong antibacterial activity against both Gram-positive and Gram-negative bacteria, and the ability of it to repair infected skin was further investigated in a rat model of Staphylococcus aureus infection. The PAD series hydrogels showed considerable antimicrobial properties and promoted the regeneration of damaged tissues in vivo, suggesting that it can be used as a multifunctional dressing and holds great promise in healing bacteria-infected skin wounds.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Donghui Kou,Tan Shi,Lei Gao,Shufen Zhang,Wei Ma
Structural colors, offering high brightness, extraordinary lightfastness, and sensitive responsiveness, are highly valuable for chromatic engineering but are bottlenecked by intricate manufacturing protocols for sophisticated nanostructures and several existing unmet issues from pragmatic uses. Herein, a versatile submicron “soap bubble” with angle-independent color and ultrasensitive responsiveness is subtly designed and fabricated as a smart structural color pigment (SCP) through a facile and scalable fabrication strategy. Each SCP consists of a porous and durable TiO2 spherical shell with in situ formed black carbons attached to its inner wall, featuring robust light, thermal, chemical, and mechanical stability and independently reflecting colors from thin-film interference. The color hue and saturation are finely tunable, which can be further mixed to enrich the variety. The SCP dispersions can serve as paints for imparting vibrant hues to automobiles, buildings, and industrial equipment, boasting exceptional coloring stability, and also be used as inks for printing and writing high-resolution vivid text on paper with excellent friction and water resistance. With refractive index-induced, reversible, and ultrasensitive (<0.2 s) colorimetric responses, the SCP is well-suited for real-time monitoring of fluid leakage in chemical production environments and unlocks new avenues in advanced sensing technologies.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Jianyao Liu,Shuo Wang,Huiling Chen,Xinlai Zhou,Dongju Chen,Zhizhang Yuan,Xianfeng Li
Polyvinylidene fluoride (PVDF) membranes are widely used in energy-related devices, such as flow batteries and osmotic energy capture. However, most PVDF-based membranes are intrinsically hydrophobic, which leads to a low conductivity. Here, we use a moderate strategy to graft hydrophilic sodium p-styrenesulfonate (NaSS) in PVDF membranes from the surface into the interior, enabling ion-accessible regions to form within the membranes. By creating and optimizing nanoscale pores in PVDF membranes to allow NaSS and redox mediation systems to diffuse into the membrane, the grafting reaction between NaSS and PVDF from outside to inside can be realized at temperate temperatures (35 °C–45 °C), which favors maintaining membrane stability. Through adjustment to the grafting degree, we can tailor the ion transport channels to obtain membranes with different conductivities. Using the methylene blue (MB)–vanadium flow battery for exemplification, our membranes enable the battery to afford a Coulombic efficiency of 99.94% and a voltage efficiency of 87.55% at a current density of 40 mA cm–2, which is significantly higher than that of the battery using a Nafion 212 membrane (CE ∼ 99.74%, VE ∼ 75.08%). Our strategy is simple and moderate and provides an efficient way to create hydrophilic ion transport channels within hydrophobic membranes.
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ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Chunhan Li,Yuanhang Wei,Xinwei Li,Peng Jiang,Xuran Dong,Qunqun Guo,Qingguo Xu,Xiyue Cao,Jianfei Xia,Zonghua Wang
Circular RNA (circRNA), a covalently closed RNA molecule, has demonstrated significant potential as a new emerging biomarker in the field of liquid biopsy due to its unique stability, tissue-specific expression patterns, and dysregulated expression in various diseases. However, the accurate quantification of circRNAs is still a tough problem because of homologous linear RNA influence, low-expression abundance, and concomitant interference in blood. Therefore, in this study, a nanobiosensor integrated with catalytic hairpin assembly (CHA) cascade amplification and magnetic control depuration, which can analyze circRNA expressed in human tissue and blood, was reported. The CHA cascade amplification is achieved by coupling the CHA reaction with subsequent formation of G-quadruplex-hemin DNAzymes, resulting in a remarkable enhancement in specificity and sensitivity. The robustness of the nanobiosensor in tissue and blood samples is supported by magnetic-driven transfer of oligonucleotide probes from the complex biological matrix after target recognition. As a proof of concept, the nanobiosensor was designed and fabricated to detect cSMARCA5, a kind of circRNA highly associated with the occurrence of hepatocellular carcinoma. The nanobiosensor exhibits a broad linear range from 10 fM to 100 nM, with a detection limit as low as 1.93 fM. Furthermore, in clinical validation experiments, the nanobiosensor successfully reveals the expression levels of cSMARCA5 in liver tissue and whole blood samples, from which hepatocellular carcinoma patients are accurately screened out among normal people, thereby providing a highly promising circulating RNA-based liquid biopsy tool with significant potential for clinical application.
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ANALYTICAL CHEMISTRY
·
2025
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IF 6.7
Haijiao Peng,Yaze Chen,Ke Shi,Kun Li,Ruidong Chen,Yuhao Liu,Chao Lu
It is important to probe the formation of metal–organic cages (MOCs) to ensure their versatility. Currently, the formation of MOCs is commonly characterized by using single-crystal X-ray diffraction, mass spectrometry, and nuclear magnetic resonance. However, the application scopes of these techniques are limited because they require that MOCs have high-quality single crystals, excellent solubility, and superior stability. In this work, we introduced an electrochemiluminescence (ECL) method to rapidly probe the formation of palladium-based MOCs. It was demonstrated that the formation of the Pd2L4 MOCs could lead to a significant increase in charge transfer resistance and a noticeable change in surface charge, resulting in substantial quenching (up to 99.1%) of the ECL signal in the Ru(bpy)32+/tripropylamine (TPA) system. This innovative “signal-off” ECL sensing mechanism allowed for a fast and ultrasensitive identification of MOC formation. Our findings not only provide a robust strategy for rapid characterization of supramolecular assemblies but also open new avenues for extending ECL-based analytical techniques to the study of other crystalline materials.
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