TALANTA
·
2019
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IF 4.916
Yiqiong Chen,Xinyue Ding,Dandan Zhu,Xucong Lin,Zenghong Xie
Nonspecific adsorption is a challenge of specific recognition on aptamer-based affinity monoliths. Here, a novel highly hydrophilic polyhedral oligomeric silsesquioxane (POSS)-containing aptamer-based hybrid-silica affinity monolith with a good recognition nature was prepared and used for specific discrimination of ochratoxin A (OTA). A homogeneous polymerization mixture consisted of POSS chemicals, hydrophilic monomers and aptamer solution was directly polymerized via the “one-pot” method. Preparation and characterization of the resultant affinity monolith were studied in detail. A highly hydrophilic nature was obtained and the typical hydrophilic interaction liquid chromatography (HILIC) was observed when acetonitrile (ACN) content in mobile phase was 25%, which reached the highest hydrophilicity of POSS-based hybrid monoliths. By using OTA as model analyte, the nonspecific adsorption was effectively suppressed. The recovery of the analogue ochratoxin B (OTB) was only about 0.1% even if the content of OTB was 50 times more than OTA, which was much better than other POSS-containing monoliths and polar siloxane-based hybrid monoliths. Applied to beer samples, the adsorption of background materials was drastically resisted, and efficient recognition of OTA was obtained with the recoveries of 94.9–99.8%. Much less disturbance was observed than that occurred in hydrophobic POSS-based affinity monolith. It lights an attractive implement with high hydrophilicity and specificity for online selective recognition of OTA.
研究领域:
分析化学
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食品科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2025
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IF 2.1
Bin Ou,Xiaofang Li,Lemei Huang,Yujiang Ke,Chaohui Che,Xiaobing Liu,Yajun Li,Kui Wu
The solubility of 2-chlorocinnamic acid in 16 pure organic solvents, including alcohols, esters, ketones, toluene, and acetonitrile, was determined by the gravimetric method at 272.15–321.55 K under 101.3 kPa. Results showed that solubility of 2-chlorocinnamic acid increased with temperature in all solvents. To correlate the experimental data, five thermodynamic models, i.e., the modified Apelblat, Buchowski–Ksiazaczak λh, NRTL, Wilson, and Yaws equations, were employed. Model accuracy was evaluated using average relative deviation (ARD) and root-mean-square deviation (RMSD), and all models provided satisfactory correlations. In addition, electrostatic potential energy surface analysis was carried out to preliminarily assess possible solute–solvent interactions, while density functional theory (DFT) calculations were used to further examine molecular interactions during dissolution. The Kamlet–Abboud–Taft linear solvation energy relationship (KAT-LSER) model was applied to analyze solvent effects. Thermodynamic functions, including enthalpy, entropy, and Gibbs free energy of mixing, were calculated using the Wilson model. The results revealed that the dissolution of 2-chlorocinnamic acid in the studied solvents is an endothermic, entropy-driven, and spontaneous process, indicating favorable solute–solvent interactions and enhanced solubility at higher temperatures.
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高影响因子
Catalysis Science & Technology
·
2025
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IF 4.2
Yu-Le Wang,Songhai Wu,Yu-Zhen Xu,Yu-Dong Shan,Yong Liu,Xu Han
The selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) using O2 remains challenging due to low epoxidation selectivity. In this work, a series of Mo-doped TS-1 (Mo-TS-1) catalysts were successfully synthesized for the epoxidation of Cy under solvent- and initiator-free conditions with O2 as the oxidant. Among them, 5Mo-TS-1 exhibited high catalytic performance, achieving 43.5% Cy conversion and 50.6% selectivity toward Cy-ep. Additionally, valuable byproducts such as 2-cyclohexen-1-ol (Cy-ol) and 2-cyclohexen-1-one (Cy-one) were obtained with yields of 28.0% and 21.4%, respectively. Since both Cy-ol and Cy-one are valuable intermediates in fragrance synthesis, over 43.5% of Cy was effectively converted into high-value products. Quenching experiments and Raman spectroscopy revealed that surface oxygen vacancies (Ov) facilitate the activation of O2 to form ≡Ov‑superoxo species, which abstract hydrogen from the allylic C-H bond of Cy to generate 3-cyclohexenyl radicals (Cy•). These radicals subsequently react with O2 to form Cy-OO•, followed by hydrogen abstraction from another Cy molecule to yield 2-cyclohexene-1-hydroperoxide (Cy-OOH). A positive correlation between Cy-OOH and Cy-ep formation underscores the critical role of Cy-OOH in the epoxidation process. Furthermore, Raman spectroscopy confirmed the presence of ≡Mo-(η2-O2) peroxo species on the catalyst surface, which preferentially attack the C=C bond of Cy to form Cy-ep. DFT calculations elucidated two distinct O2 activation pathways: In Pathway I, O2 is activated at Ov sites to form ≡Ov‑superoxo, which subsequently reacts with Cy to generate ≡Ov‑peroxo, Cy-OOH, and Cy•. In Pathway II, Mo(V/VI) sites either directly activate O2 or react with peroxo intermediates (≡Ov‑peroxo or Cy-OOH) to form ≡Mo-(η2-O2). This species selectively epoxidizes the alkene bond in Cy to Cy-ep. Notably, the direct activation of O2 at Mo(V/VI) sites bypasses the allylic oxidation route, thereby enhancing the epoxidation selectivity beyond the theoretical limit of 50.0%. This study provides new insight on the importance of surface superoxo and peroxo mediated by Ov and Mo(V/VI) in the epoxidation processes.
研究领域:
催化化学
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材料化学
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绿色化学
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多相催化
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氧化反应
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Tingting Jiang,Siyu Huang,Yu Wang,Guanbo Wang,Wei Wang,Haifeng Zhang
Persulft-based advanced oxidation processes (PS-AOPs) are an efficient strategy to degrade refractory pollutants. Fabricating a highly efficient catalyst is the most pivotal factor in PS activation. This study designs a novel CoP 3 -anchored layered Bi 2 O 2 S through an interface engineering strategy, where the unique electronic structure and surface properties of Bi 2 O 2 S lead to dramatically reduced cobalt ion leaching compared with that of CoP 3 . It exhibited outstanding catalytic activity and achieved nearly complete removal (>99%) of 50 mg L −1 2,4-Dichlorophenol (2,4-DCP) within 30 min. Radical quenching experiments, EPR technique, electrochemical tests, and HPLC validated the coexistence of radical (•OH, SO 4 •− ) and non-radical ( 1 O 2 , electron transfer, high-valent metal species) pathways in the Light/Bi 2 O 2 S/CoP 3 /PMS system for 2,4-DCP degradation. Importantly, Bi 2 O 2 S/CoP 3 induced a pronounced photothermal effect that enhanced 2,4-DCP degradation efficiency. Furthermore, the attack sites of 2,4-DCP were precisely identified based on the Fukui index. Based on density functional theory calculation and high-performance liquid chromatography-mass spectrometry, the detailed degradation pathways were proposed. The toxicity of 2,4-DCP and its intermediate products were predicted by using the toxicity assessment software tool. Moreover, excellent reusability, real-water treatment efficacy (verified by 3D-EEM), high-efficiency removal of multiple pollutants, and wide pH adaptability (3−11) confirm practical potential for sewage treatment. This study provides insight into designing a highly efficient and green catalyst for simultaneous pollutant treatment.
研究领域:
环境催化
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材料科学
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水处理技术
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高级氧化过程
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纳米材料
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理论化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Min Zhou,Shuming Hong,Bo Jin,Min Xiao,Haiyan Zhang,Zhiwu Liang,Hongxia Gao
Liquid-liquid phase-separation absorbents demonstrate promising potential for enhancing CO 2 capture performance and reducing regeneration energy consumption. This work studied N , N -dimethylethylenediaminebased (2DMEDA)-physical solvents-H 2 O systems to evaluate their phase separation behaviors and absorption-desorption performance and developed a new liquid-liquid phase separation absorbent based on a 2DMEDA-sulfolane (SUL)-H 2 O system. Phase separation absorbent with varying 2DMEDA-SUL-H 2 O ratios were evaluated for phase separation behavior, viscosity and absorption-desorption properties. When the 2DMEDA-SUL-H 2 O system was formulated at 30:35:35 mass ratio, it demonstrated a relatively low dynamic viscosity of 20.14 mPa·s and a CO 2 cyclic capacity of 1.83 mol/L which was 1.44 times that of 30 wt% MEA aqueous solution. 13 C NMR analyses suggest that carbamates, bicarbonates and free amines predominantly concentrate in the CO 2 -rich phase, while SUL is primarily located in the CO 2 -lean phase. Furthermore, the phase separation mechanism was elucidated through density functional theory (DFT) calculations at the B3LYP/6–311++G(d,p) level and molecular dynamics (MD) simulations. It indicated that the formation of highly polar products and hydrogen bonding interactions among components were characterized as key contributing factors, and MD simulations further manifest aggregation propensities between reaction products and water molecules, driving spontaneous separation into CO 2 -rich and CO 2 -lean phases.
研究领域:
化学工程
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碳捕集与封存
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分离科学
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计算化学
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环境技术
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Jianwei Luo,Yingsi Huang,Xinghai Huang,Jinyun Cai,Haiyi Zhong
Emphasizing the use of biomass resources is a vital step in advancing green chemistry and environmental protection, significantly contributing to the reduction of carbon emissions and the promotion of carbon neutrality. Converting agricultural waste into biomass resources, such as nanocellulose, is of great significance for a low-carbon economy. Furthermore, the challenge of environmentally friendly and selective separation of natural active plant ingredients still needs to be addressed. In this study, drawing inspiration from the wisdom of “Pods burned to cook peas”, the biomass of the nonmedicinal portion of the herbal medicine (Sophora tonkinensis Gagnep.) was processed to obtain nanocellulose for the preparation of a magnetic molecularly imprinted composite, which was used to separate quercetin from the medicinal portion of this herbal medicine. The stacked complex of magnetic Fe3O4 nanoparticles and nanocellulose particles served as the carrier, and the magnetic nanocellulose molecularly imprinted polymer (MIPs/MCNC) was prepared through surface imprinting. It exhibited a strong adsorption capacity (Qe = 50.64 mg/g) and imprinting factor (IF = 2.55) as well as specific selectivity (Ks’ = 3.48) against structurally similar compounds (naringenin). The regeneration capability remained at 75% after 5 adsorption-elution cycles. It was also successfully applied in a complex solvent environment to selectively separate quercetin from the deep eutectic solvent (DES, choline chloride─acrylic acid) extract of S. tonkinensis Gagnep. Additionally, an interdisciplinary approach was integrated into the design process of MIPs/MCNC, utilizing density functional theory (DFT) to effectively guide the design of functional monomers. This work presented a concept with significant potential for reusing the nonmedicinal parts waste of herbal medicine as nanocellulose and for the environmentally friendly and selective separation of active components.
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2025
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IF 7
Yi Yi,Pengxiang Zhang,Yixin Shen,Junhui Tan,Bao-Wen Li
Solution-processable high-k perovskite nanosheets show considerable potential for applications in printed electronics due to their unique structural properties and exceptional physical characteristics. However, their dispersibility and compatibility in various organic solvents remain insufficiently understood, with a lack of systematic investigation, which restricts their broader application potential. In this study, the dispersion behavior of high-k perovskite nanosheets, specifically Ca2Nb3O10 (CNO) and Ca2NaNb4O13 (CNNO), was examined in 20 different organic solvents. By correlating the physicochemical properties of these solvents, including surface tension, dielectric constant, and empirical solvent parameters, with Hildebrand and Hansen solubility models, we identified the underlying solvent–nanosheet interaction mechanisms responsible for dispersion stability. Polar protic solvents, such as water and methanol (MeOH), as well as polar aprotic solvents, like dimethyl sulfoxide (DMSO), acetonitrile (ACN), N,N-dimethylformamide (DMF), propylene carbonate (PC), and N-methyl-2-pyrrolidone (NMP), facilitate uniform and stable nanosheet dispersions. These solvents promote dispersion stability through strong dipole–dipole interactions and moderate surface tension matching. Based on these findings, we developed a series of organic solvent-based inks incorporating high-k perovskite nanosheets, demonstrating excellent printing adaptability for electrical device fabrication, and achieving stable device performance. This work provides a comprehensive library of organic solvents that effectively disperse high-k perovskite nanosheets, thereby broadening their potential applications in printed electronic devices.
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Weifang Zhang,Lianyang Huang,Weijing Guo,Yuan Cheng,Menglu Zhang,Aristides Bakandritsos,Radek Zbořil,Chunli Wang
In Fenton-like reactions, the elevation of the spin state of transition metals enhances the redox processes of adsorbed peroxides and improves the oxidative performance. This study reports an easily accessible carbon-supported high-spin cobalt cluster, Co–NCs/C, which demonstrates enhanced kinetics through selective high-valent cobalt-oxo species (Co(IV)═O) generation for peroxymonosulfate (PMS)-induced catalytic oxidation. This catalyst achieves rapid degradation of sulfamethoxazole (SMX) within the modified kinetic rate constant (k-value) of 2001.7, surpassing all previously reported Co-based catalysts. Furthermore, combined experimental characterizations and density functional theory calculations demonstrate the stable size distribution of cobalt clusters anchored on carbon supports. Within a broad size distribution (0–6 nm), these clusters consistently retain high-spin configurations and exhibit excellent catalytic performance in SMX degradation. The tailored electronic structure of the high-spin Co sites enhances the adsorption and activation of PMS, thereby accelerating the degradation process. This work provides a practical and cost-effective strategy for designing high-efficiency catalysts for PMS-based advanced oxidation processes.
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DOI
PubMed
高影响因子
ACS Omega
·
2025
·
IF 4.3
Ramarajan Ramanathan,Ashish Kumar,Himamaheswara Rao,Raj Kumar Samudrala
Researchers are actively investigating cost-effective, indium-free n-type transparent conducting oxides (TCOs) for optoelectronic applications. Silver-doped SnO2 (ASO) thin films, fabricated via spray deposition, serve as promising alternative electrodes for dye-sensitized solar cells (DSSCs), where Ag doping optimizes the electrical and optical properties. The structural, morphological, optical, and electrical transport properties of the as-deposited ASO thin films were analyzed using X-ray diffraction, field-emission scanning electron microscopy, X-ray photoelectron spectroscopy, UV–vis spectroscopy, and Hall effect measurements to assess phase composition, surface morphology, elemental states, optical behavior, and charge transport characteristics. At 0.4 wt % Ag (ASO4), the film exhibits 88.7% transmittance in the visible range, a wide bandgap of 3.73 eV, and low resistivity (4.26 × 10–4 Ω cm) with a sheet resistance of 18.6 Ω/□, making it a superior TCO candidate. To understand charge transport mechanisms, Arrhenius analysis was used to determine activation energies, while a four-probe method revealed resistance stability up to 400 °C. The power conversion efficiency (PCE) of the DSSC device was effectively optimized using ASO electrodes, where varying Ag concentrations played a crucial role in enhancing efficiency. Notably, the ASO4 film demonstrated a remarkable PCE of 4.69%. Integrating ASO electrodes into DSSCs yielded enhanced PCE, reinforcing their viability as a cost-effective replacement for ITO/FTO electrodes in the next-generation solar technology.
研究领域:
材料科学
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光伏技术
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薄膜技术
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光电子学
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纳米材料
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Shufang Zhao,Xiaojie Wu,Nannan Wang,Xian Zhou,Xiangxiang Chen,Ying Tang,Xin Tang,Lili Lin,Siyu Yao
Photocatalytic valorization of lignin, featuring the selective cleavage of lignin linkages and subsequent upgrading of resulting monomers, is an emerging and promising approach for utilizing this natural renewable aromatic polymer. However, existing photocatalytic conversion strategies typically perform singular functions (either depolymerization or monomer upgrading) and face pronounced separation challenges since phenolic and acetophenone intermediates derived from lignin monomers often exhibit similar physical properties. This work introduces a domino conversion strategy combining lignin β–O–4 dimer cleavage and acetophenone dimerization using a ZnS/Zn2In2S4 composite photocatalyst constructed via a light-induced phase segregation method. The ZnS/Zn2In2S4 composite exhibits synergistically enhanced redox capability and charge separation, enabling hole-driven Cβ–O scission and electron-mediated pinacol coupling of acetophenone under mild conditions. This approach achieves near-quantitative conversion of acetophenone to C16+ vicinal diols (biodiesel precursors) along with phenolic monomers. Scalable reactions demonstrate 91% phenolic and 90% C16+ yields after hydro-deoxygenation, circumventing distillation-based separation. The integrated strategy presents an efficient, step-economical route for coproducing value-added aromatics and biofuels, advancing photocatalytic lignin valorization.
研究领域:
光催化
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木质素高值化
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可再生能源
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绿色化学
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生物质转化
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产品关联
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Qianqian Wang,Wenxin Bian,Junjie Si,Feng Ding,Zichen Zhao,Bo Hu,Kaihang Wang,Jiefu Tan,Desui Chen,Sunan Xu,Tenglong Sun,Muzhi Cai,Zugang Liu
Lead halide perovskites are promising materials for high-performance light-emitting diodes (LEDs) owing to their optoelectronic properties, including high photoluminescence quantum yield (PLQY), tunable bandgap, and outstanding charge carrier mobility. Despite rapid progress, achieving high luminance at a low operating voltage remains a major challenge for perovskite LEDs (PeLEDs), largely due to limited carrier injection in conventional device architectures. Here, we present a synergistic strategy to realize low-voltage, high-efficiency PeLEDs. The device integrates a [2-(3,6-dibromo-9H-carbazol-9-yl)ethyl]phosphonic acid (Br-2PACz) self-assembled monolayer, a compact three-dimensional (3D) perovskite emissive film, and a zinc oxide (ZnO) electron transport layer (ETL). Sulfobetaine 10 (SFB) is employed to regulate crystallization, leading to dense and uniform perovskite films with reduced trap density. The Br-2PACz interlayer simultaneously passivates interfacial defects, facilitates hole injection, and suppresses electron leakage by tuning the energy levels. In addition, the high-mobility ZnO ETL ensures efficient electron injection. The optimized PeLED exhibits a low turn-on voltage of 1.9 V and achieves a luminance of 39,000 cd m–2 and a current density of 38.5 mA cm–2 at 2.5 V. The device delivers a peak external quantum efficiency (EQE) of 22.5% and a peak power efficiency (PE) of 128.7 lm W–1. Moreover, this strategy demonstrates good scalability: large-area PeLEDs (1600 mm2) retain a competitive EQE of 11.2% with uniform emission. This work supplements the research on energy-efficient, low-voltage-operating, and scalable PeLEDs.
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PubMed
高影响因子
Frontiers in Nutrition
·
2025
·
IF 5.1
Jing Li,Caiyan Jiang,Yan Liu,Xiaoqing Miao,Pengfei Jiang
This research primarily examines the effects of three thermal processes–air frying, water steaming, and oil frying–on the volatile and non-volatile flavor compounds of salted Spanish mackerel dried meat (with a salt concentration of 6% and drying durations of 4 and 6 days). The results indicated that 45 volatile flavor compounds were discovered using GC-IMS, with the oil frying group exhibiting the highest concentration of desirable volatiles. The e-tongue findings indicated that the savory flavor was the most prominent across all sample groups. According to LC-MS measurement of free amino acid content, the concentration of fresh flavor amino acids was most pronounced in the oil frying group. The oil frying group also earned the highest overall rating in the sensory evaluation. This research provides a theoretical framework for the development of prepared meals with salted and dried Spanish mackerel.
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）