ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Lei Ge,Jiaqi Li,Gaojing Du,Kai Sheng,Jingwei Hou,Binyu Zhou,Yatao Zhang,Bart Van der Bruggen,Junyong Zhu
Microporous membranes featuring 3D nanochannels present a compelling avenue for energy-efficient liquid separations, attributable to their tunable interconnected through-pore structures. However, the rational design of 3D-nanochannel membranes that simultaneously achieve high permeance and selectivity remains a challenge, arising from the scarcity of appropriate molecular building blocks and the reliance on empirical synthetic methods. Herein, an innovative 3D polyacylhydrazone (PAH) membrane with unique pore-interconnected structures is constructed on a porous hydrogel using contorted tetrahedral aldehydes (TFS) monomers via an in situ interface-confined strategy. Manipulation of side alkyl chain lengths within terephthalohydrazide (TPH) derivates enabled the enhancement of microporosity and tunable pore environment of PAH nanofilms. Molecular dynamics simulations revealed that TPH EO linkers with higher reactivity and moderate steric hindrance facilitate superior pore interconnectivity and sharpened pore size distributions. The resulting PAH membranes achieved exceptional methanol permeances of 10.1 L m −2 h −1 bar −1 and small molecular weight cut-offs of 310 Da, outperforming the state-of-the-art polyamide membranes. This further translated into an outstanding capability in the fractionation of active pharmaceutical ingredients within organic solvent systems. This work demonstrates the efficacy of rational molecular design in developing high-microporosity membranes with tailored interconnected nanochannels, underscoring the potential of 3D microporous membranes for accurate molecular separations.
研究领域:
材料科学
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分离技术
·
化学工程
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产品关联
DOI
高影响因子
Polymer Chemistry
·
2024
·Vol. 15
·期 22
·2253-2264
·
IF 4.1
Yunsheng Xu,Chonglin Liu,Yanying Zhao,Xianming Zhang,Minna Hakkarainen
Acylhydrazone linkages are appealing for the design of covalent adaptable networks (CANs) due to their reversible nature and ease of formation from readily available starting materials. However, acylhydrazone CANs typically exhibit dynamic behavior within a limited temperature range due to their slow exchange rate. Here, vanillin was modified by a two-step reaction involving allylation and imination, followed by photo-curing with a four-armed thiol to fabricate acylhydrazone CANs. The dynamic behavior of these CANs could be controlled by adjusting the amount of p-anisidine (AD) organocatalyst. A model compound reaction revealed that the addition of a catalyst transforms the mechanism of acylhydrazone exchange from a 2 + 2 cycloaddition reaction to a nucleophilic addition reaction, effectively lowering the energy barrier of the intermediate state. CANs with higher amounts of AD catalyst exhibited shorter relaxation times and lower activation energies, thereby expanding the reprocessing temperature window and enhancing the recovery ratio of tensile stress after reprocessing. All the fabricated CANs demonstrated ready chemical recyclability in acidic or AD/DMSO solutions at 80 °C, following two different mechanisms depending on the reaction medium. These findings pave the way to photo-curable renewable acylhydrazone CANs with adjustable viscoelastic properties and mechanical and chemical recyclability enabled by rapid dynamic exchange reactions.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2025
·Vol. 26
·期 7
·3231
·
IF 4.9
Xin Lin,Hua Liang,Ke Dai,Jing Zhou,Qiang Tian,Yuge Xiang,Zhicheng Guo,László Almásy
Thorium is a notable candidate for resolving uranium shortage caused by the global application of nuclear power generation. Uranium extraction from seawater is another attempt to handle its source deficiency, however, vanadium is one of the main competitive elements in that process. Exploration of probes which can discriminatively detect thorium and vanadium from uranium has primary significance for their further separation and for environmental protection. Herein, N′-(2,4-dihydroxybenzylidene)-4-hydroxylphenylhydrazide,AOH, is used as sensor for Th4+and vanadyl (VO2+) determination.AOHdemonstrates a specific “turn-on” fluorescence selectivity towards Th4+over f-block and other foreign metal ions, with a detection limit (LOD) of 7.19 nM in acidic solution and a binding constant of 9.97 × 109M−2. Meanwhile, it shows a “turn-off” fluorescence response towards VO2+over other metal ions at the coexistence of Th4+, with a LOD of 0.386 μM in the same media and a binding constant of 4.54 × 104M−1. The recognition mechanism, based on HRMS,1H NMR, and FT-IR results, demonstrates that VO2+causes the fluorescence quenching by replacing Th4+to coordinate withAOH. In real water detection tests, Th4+and VO2+exhibited satisfying recoveries. These findings expand the application of sensors in nuclide pollution control.
研究领域:
分析化学
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环境科学
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DOI
PubMed
高影响因子
Desalination and Water Treatment
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2024
·
IF 1
You-qun Wang,De-jun Zeng,Xiao-hong Cao,Yin Dai,Hui-jie Ma,Yun-hai Liu,Zhi-bin Zhang
In this work, the functional group of salophen with high affinity to U(VI) was grafted to hydrothermal carbon spheres (HCSs) to improve the adsorptive ability for U(VI). Through the application of scanning electron microscopy, Fourier transform infrared, and zeta potential measurement, the micro-morphology, functional group, and surface charge of the adsorbents was characterized. Comprehensive investigation of the factors affected U(VI) adsorbed by HCSs and salophen group modified HCSs (HCSs-sal) were conducted. Different types of kinetic and thermodynamic models were utilized to explore the adsorption processes. The results of this study, indicated that the adsorption of U(VI) on HCSs-sal fitted well to Langmuir equations with the monolayer capacity of 332.51 mg g –1 . Furthermore, the adsorptive selectivity of HCSs for U(VI) was also remarkably enhanced after functionalization with the salophen group. Overall, HCSs-sal appears to have the potential to be a prospective candidate for the selective adsorption of U(VI).
研究领域:
环境科学
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材料科学
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核化学
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水处理技术
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2019
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IF 2.12
Zhenyuan Yang,Daqiang Wu,Ke Dai,Shiquan Cao,Zongchen Li,Heyan Huang,Zhibin Shang,Hua Liang,Minhao Yan,Suyuan Xie
As Al 3+ is detrimental both to human and other organisms, a simple sensor, acylhydrazone AhzF , is synthesized in one step and its structure is confirmed by single crystal X-ray diffraction. AhzF shows specific fluorescence turn-on response for Al 3+ over other metal ions at UV 365 nm, observed by naked-eyes. Its detection limit can reach to 1.11 × 10 −9 M in ethanol. Meanwhile, AhzF at low concentration can detect Al 3+ with excellent interference resistance to typical disturbing metal ions including Cu 2+ and Fe 3+ . For the first time, concentration influence of Fe 3+ during AhzF detecting Al 3+ has been explored and it has been found that the fluorescence of AhzF-Al 3+ is partly quenched by Fe 3+ while with no influence by Cu 2+ at high concentration (above 10 −6 M), indicating its good low concentration advantage during Al 3+ detection. The binding mode exhibits a 1:1 M ratio between AhzF and Al 3+ , which are confirmed by titration test, Job’s plot, 1 H NMR spectra and mass spectrum . It also exhibits good reusability by alternate addition of Al 3+ and EDTA to the AhzF solution. The pH effect tests suggest its good sensitivity from pH 4 to pH 10 and AhzF can recognize labeled Al 3+ in tap water directly by naked eyes, which makes it possible for the application in real environment.
研究领域:
化学传感器
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环境科学
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分析化学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Shengmao Chao,Chiara Valsecchi,Ji Sun,Hong Shao,Xinxia Li,Changyu Tang,Meikun Fan
The spontaneous generation of hydrogen peroxide (H2O2) within atmospheric microdroplets, such as raindrops and aerosols, plays a crucial role in various environmental processes including pollutant degradation and oxidative stress. However, quantifying hydroxyl radicals (•OH), essential for H2O2 formation, remains challenging due to their short lifespan and low concentration. This study addresses this gap by presenting a highly sensitive and selective surface-enhanced Raman scattering (SERS) nanosensor specifically designed for quantifying •OH within water microdroplets. Utilizing a phthalhydrazide (Phth) probe, the SERS technique enables rapid, interference-free detection of •OH at nanomolar concentrations. It achieves a linear detection range from 2 nM to 2 μM and a limit of detection as low as 0.34 nM. Importantly, the SERS sensor demonstrates robustness and accuracy within water microdroplets, paving the way for comprehensive mechanistic studies of H2O2 generation in the atmosphere. This innovative approach not only offers a powerful tool for environmental research but also holds potential for advancing our understanding of atmospheric H2O2 formation and its impact on air quality and pollutant degradation.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 32
·期 10
·e4483
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IF 3.581
Xufeng Wu,Lingyu Li,Wenlong Jiang,Lihong Zhou,Qingle Zeng
Tosylhydrazones are a kind of labile and highly reactive compounds, which are apt to be transformed into reactive diazo compounds and then into extremely reactive carbenes under the basic condition. In order to fulfil the valuable C-N coupling reaction, diaryliodonium salts are evaluated and prove to be a class of efficient electrophiles. The reaction with ligand-free copper salt as catalyst shows a wide range of substrate scope. A plausible mechanism is proposed.
研究领域:
有机化学
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合成化学
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 20
·52144
·
IF 3.057
Jingyu Ren,Xiangbin Dong,Yanjie Duan,Lin Lin,Xiaowei Xu,Jichao Shi,Runping Jia,Dandan Wu,Xinyao He
A series of self-healing waterborne polyurethane (WPU) films utilizing reversible covalent bond acylhydrazones diol (PA) as chain extender were successfully synthesized. The self-healing performance of WPU with different content of chain extender PA has been systemically characterized via cut-and-healing tests and mechanical quantitative evaluation. The film can repair cracks through acylhydrazone exchange reactions within 12 h. When the content of PA is 1.5 wt%, the WPU has the highest self-healing efficiency of 90.5%. Meanwhile, the effect of PA mass fraction on the particle size distribution, mechanical ability, crystallization, water resistance properties, and thermal stability of WPU were evaluated. With the introduction of acylhydrazone bonds, the hydrophobicity of the WPU material was enhanced, while achieving self-healing performance, which solves the problem of aging and replacement of materials. These results indicated that the self-healing WPU exhibited great application prospect as a versatile material.
研究领域:
材料科学
·
高分子化学
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DOI
高影响因子
EUROPEAN POLYMER JOURNAL
·
2024
·
IF 5.8
Xiaowei Li,Chilong Liu,Xiaoru Quan,Yanxin Zhang,Su Wang,Shuangfei Zhao,Jiming Yang,Yirong Feng,Wei He,Kai Guo
Acylhydrazone linkages are attractive in designing reconfigurable and chemically recyclable polymer due to their reversible characteristics and ease of preparation. We fabricate mechanically strong, thermally stable and chemically recyclable poly(acylhydrazone)s (pDFF-IPDH) using biobased 2,5-diformylfuran (DFF) and dihydrazide compounds as monomers. The linear chains are physically cross-linked via hydrogen bonding between the acylhydrazone moieties. The pDFF-IPDH sample exhibits good mechanical properties, offering both high strength and toughness. The linear and reversible acylhydrazone backbones endow polymers with attractive temperature-dependent dynamic natures, which enables the topological network to rearrange, giving the poly(acylhydrazone)s excellent reprocessability. Moreover, the feasibility of formaldehyde-promoted depolymerization presents an effective recycling pathway, offering promising opportunities in addressing the challenge between recyclability and service performance.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 92
·50301-50311
·
IF 3.708
Caicai Lu,Bingqiang Li,Na Liu,Guolin Wu,Hui Gao,Jianbiao Ma
A pH-responsive polypeptide nanogel was prepared via hydrazone self-crosslinking under mild conditions. Zwitterionic sulfobetaine was introduced to the polypeptide by aminolysis reaction of polysuccinimide with N,N-dimethylaminopropylamine, and the subsequent ring-opening reaction between tertiary amine and 1,3-propanesultone. The hydrazine and aldehyde modified poly(α,β-L-aspartic acid) precursors, poly(aspartamide sulfobetaine-co-aspartylhydrazide) and poly(aspartamide sulfobetaine-co-2-oxoethyl aspartamide) were prepared by the successive aminolysis reaction of polysuccinimide. The obtained zwitterionic poly(aspartamide) nanogel exhibited excellent anti-protein adsorption ability and stability in protein solutions. An anticancer drug, doxorubicin (DOX), was entrapped into the nanogel, and showed accelerated release under acidic conditions. Additionally, the nanogel entrapped DOX could be successfully released into the cancer cells and showed high cytotoxicity. This easily prepared nanogel, with features of biocompatibility, anti-protein adsorption ability, and pH-responsiveness, is a promising controlled drug delivery system.
研究领域:
生物材料
·
药学
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生物医学工程
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产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Wei Zhu,Jiejuan Tang,Ling Huang
Mercury-ion pollution in water is very dangerous to human health and ecological environments. It is necessary to propose a simple, fast and low-cost testing method for mercury-ion detection. Cold atomic spectrophotometers are often used for the detection of mercury ions, but because the instruments are expensive and cumbersome to operate, the method is only suitable for laboratories. In this work, we propose a simple electrochemical method for the determination of mercury ions based on a dithizone-modified glassy carbon electrode. The dithizone modification can significantly enhance the sensing performance of the electrode. Under optimized conditions, the proposed electrochemical sensor can linearly detect Hg(II) between 0.1 and 100 μg/L with a low detection limit of 17 ng/L.
研究领域:
环境科学
·
分析化学
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DOI
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
·
2014
·
IF 2.212
Zhong-Ying Ma,Jia Shao,Wei-Guo Bao,Zhao-Yan Qiang,Jing-Yuan Xu
The preparation and the structure of a copper(II) complex, [Cu(4ML)Cl] (1) (H4ML = 2-acetylpyridine-4-methylthiosemicarbazone), are described. Complex 1 crystallizes in a monoclinic P21/c space group with a = 7.977(2) Å, b = 15.824(5) Å, c = 9.126(2) Å, α = γ = 90°, β = 91.974(2)°, V = 1151.26(5) Å3, Z = 4, F(0 0 0) = 620. According to X-ray crystallographic studies, each Cu(II) ion lies in a square planar coordination geometry based on the 4ML− and Cl− ligands. The complex displayed excellent inhibitory activity against various tumor cells (HeLa, HepG-2 and SGC-7901), offering lower IC50 value of 3.2 ± 0.7 μM than cisplatin (10 ± 2 μM) on HeLa cells at 48 h. Complex 1 could significantly suppress HeLa cell viability in a dose-dependent manner. Flow cytometric analysis showed that 1 induced HeLa cell apoptosis, which might be associated with cell cycle arrests at S and G2 phases. Consistent with results of DNA cleavage experiments, comet assay indicated that 1 caused severe DNA fragmentation. The production of ROS was elevated with increasing concentration of 1, suggesting that 1 was capable of promoting HeLa cell apoptosis through an oxidative DNA damage pathway.
研究领域:
药物化学
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肿瘤学
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生物无机化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）