RSC Advances
·
2014
·Vol. 4
·期 90
·49153-49160
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IF 3.708
Dan Liu,Nan Song,Ye-Chun Cheng,Dai-Xiong Chen,Qiong Jia,Ying-Wei Yang
Poly(glycidyl methacrylate-co-ethylene dimethacrylate) modified with a new supramolecular macrocycle, carboxylatopillar[5]arene, was successfully prepared inside a capillary. The functionalized polymer monolith material was characterized by scanning electron microscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, and Fourier-transformed infrared spectra. The experimental results showed that this type of polymer possess a good network skeleton structure and excellent extraction properties for the enrichment of parabens by polymer monolith solid-phase microextraction coupled with high performance liquid chromatography. Compared with other pre-treatment methods, the simple operation and inexpensive instrumentation characteristics of the developed polymer monolith SPME method make it more suitable for the extraction of parabens in red wine samples with great potential for further broadening its applications in the enrichment of other real samples.
研究领域:
分析化学
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环境科学
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食品安全
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材料科学
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色谱学
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2018
·Vol. 136
·期 3
·46984
·
IF 1.901
Xiaojuan Liu,Fengjing Wu,Chaktong Au,Qi Tao,Mingyu Pi,Wenhui Zhang
Molecularly imprinted polymer (MIP) for selective extraction of p -hydroxybenzoic acid ( p -HB) was synthesized by suspension polymerization using p -HB as template, 4-vinyl pyridine as functional monomer and ethylene glycol dimethacrylate as crosslinker. As characterized by scanning electron microscopy, the MIP particles are spherical, with size ranging from 1 to 8 μm. Compared with the non-imprinted polymer (NIP), the MIP shows higher binding capacity toward p -HB: maximum binding capacity for p -HB being 8.07 μmol g −1 over MIP and 3.88 μmol g −1 over NIP. The adsorption of p -HB on MIP follows the Freundlich model and displays pseudo-second-order kinetics. The results of selective and competitive binding experiments confirm that the molecularly imprinted sites have excellent recognition ability toward p -HB. The results reveal that the MIP is a promising adsorbent for selective extraction of p -HB from water samples. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 46984.
研究领域:
环境科学
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分析化学
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高分子材料
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污染物去除
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分子识别
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2025
·
IF 11.3
Yiming Sun,Chenying Zhou,Shuang Meng,Shuang Zhong,Yang Liu,Chuanshu He,Peng Zhou,Bo Lai
Heteroatom doping has been applied as an excellent method for mediating the catalytic reactivity of carbon materials. To overcome the inherent defect of slow Fe(III) reduction in Fenton chemistry, this work finds that boron-doped carbon materials demonstrate high cocatalytic activity in boosting Fenton oxidation. During Fenton chain reactions catalyzed by boron-doped reduced graphene oxide (B-rGO, the typical boron-doped carbon material), highly reactive near-free Fe(III) formed on the B-rGO surface can dramatically promote H2O2 mediated Fe(III) reduction, which strongly accelerates the rate-determining reaction in Fenton chain reactions to generate hydroxyl radicals. The results of DFT calculations, electrochemical analysis, characterizations (XAFS, in situ Raman, and HAADF-STEM), and pH-dependent performance reveal that doped boron atoms can modulate the electron-deficient iron atom of FeOH2+ by stretching the Fe–O bond (from 163.6 to 179.2 pm), which forms near-free Fe(III) on the B-rGO surface with higher oxidation capability than free Fe(III), and the Fe(III) oxidation potential is positively and linearly related to the boron content of B-rGO (R2 = 0.96). Moreover, near-free Fe(III) can dramatically oxidize H2O2 (a green electron donor) to accelerate Fe(II) regeneration, thereby promoting Fenton chain reactions for long-lasting Fenton oxidation. These discoveries afford a strategy for designing green and sustainable cocatalysts to overcome the intrinsic weaknesses of classical Fenton chemistry.
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CHEMICAL PHYSICS
·
2025
·
IF 2.4
Qiuhui Zhao,Yaqi Jing,Jiale Zhang,Jiadan Xue,Jianjun Liu,Jianyuan Qin,Zhi Hong,Yong Du
Isoniazid (INH), a frontline anti-tuberculosis drug, faces rising resistance and hepatotoxicity, motivating crystal-engineering approaches. The INH-4-hydroxybenzoic acid (INH-HBA) cocrystal shows multiple polymorphs, its hydrate exists in two forms whose lattice water markedly alters hydrogen-bond topology and molecular packing. We combined terahertz time-domain spectroscopy (THz-TDS) and FT-Raman spectroscopy with periodic solid-state DFT and potential energy distribution (PED) analysis to assign vibrational modes and link spectral features to structural motifs. Hirshfeld surface analysis indicates form I is dominated by multi-directional O H...N contacts and an R 2 2 ( 8 ) N H...O synthon that yields parallel layered packing. By contrast, form II uses lattice water to bridge O H...O/N H...O interactions and weak C H...O contacts, producing a cross-stacked three-dimensional network lacking R 2 2 ( 8 ) dimers. Observed spectral differences are attributed to these distinct intermolecular interactions and associated vibrations. By integrating experimental and theoretical data, this study provides spectroscopic-structural insights into INH-HBA hydrate polymorphism, offering a foundation for pharmaceutical cocrystal identification and design.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Min Tang,Wu Liu,Jinquan Wan,Shiyu Zuo,Zhiyong Wang,Rui Peng
Fenton-like oxidation is often hampered by high energy barriers, uncontrolled oxidation pathways, and inefficient reactive oxygen species (ROS) utilization. Here, we report an energy-driven confined catalytic nanoreactor that leverages the in-situ confinement energy generated within nanopores to fundamentally regulate degradation thermodynamics. Taking sulfamethoxazole (SMX) as a model contaminant, the confined nanoreactor exhibited a 22.11-fold higher kinetic constant (0.157 min −1 ) and 40 % enhanced mineralization efficiency compared with its non-confined system. The imprinting channel of confined nanoreactor enabled selective adsorption of SMX within the nanochannel, inducing pronounced confinement effects. The resulting confinement energy triggered a low-entropy degradation pathway (ΔS reduced by 3.2 × 10 3 -fold), which broke thermal equilibrium constraints and redirected SMX oxidation along a low-energy-barrier route. The in-situ confinement-induced low-entropy reaction not only accelerated pollutant degradation but also improved ROS conversion efficiency. This study demonstrated a green and sustainable approach to overcome the intrinsic efficiency bottleneck of Fenton-like processes and provide a new perspective on exploiting nanoconfinement effects for environmental remediation.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2026
·
IF 6.7
Mingzhu Zhang,Ke Wang,Guoli Li,Xinlu Bao,Kebin Ye,Aoyun Cui,Jishuang Zhang,Lin Zhou
Photodegradation-targeting chimeras (PDTACs) addresses the off-target toxicity issues of proteolysis-targeting chimeras (PROTACs) in terms of technical principle; Difficulty in defining tumor boundaries and controlling light exposure increases the risk of damaging peritumoral tissues if light exposure oversteps the tumor. This study discovered that compared to SV-HUC-1 cells (normal cells), Von Hippel-Lindau (VHL) exhibits more active regulation of CDK2/4 in T24 cells (bladder cancer cells); Based on this, a series of PDTACs linking VHL ligands to photosensitizers were synthesized, and ZnPc-PEG 2 -VH032 was selected as the most potent antitumor compound. This compound degrades VHL upon light exposure and, when combined with photodynamic therapy (PDT), efficiently kills T24 cells with a phototoxicity index (PI) of 36,397. More importantly, after illumination, ZnPc-PEG 2 -VH032 exhibited a selectivity index (SI) of 749 for killing T24 cells versus SV-HUC-1 cells, achieving selective tumor cell targeting under light conditions and effectively mitigating the risk of damage to peritumoral tissues. This study demonstrates the potential of VHL as a precision therapeutic target for tumors and identifies the first PDTAC drug characterized by high PI and SI. It provides novel insights and structural references for developing drugs that selectively kill tumor cells.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Wenbo Yang,Chengming Xiao,Yuxin Tian,Yunlong Wang,Junwen Qi,Yujun Zhou,Zhigao Zhu,Yue Yang,Jiansheng Li
While the significance of the coordination microenvironment in single-atom catalysts (SACs) is well recognized, precise modulation of the more extended coordination sphere remains a substantial challenge. Herein, a series of cobalt-based SACs (Co/TpHz, Co/TpPa, Co/TpBD) were fabricated via a secondary coordination sphere (SCS) modulation strategy. This was achieved by anchoring isolated Co sites into three β-ketoenamine-linked covalent organic frameworks (COFs) with tailored conjugation degrees in their frameworks, which resulted from the controlled variation in the number of aromatic rings within the aminobenzene-based linkers. Remarkably, the monobenzene-type Co/TpPa catalyst exhibited superior performance in the removal of bisphenol A via Peroxymonosulfate (PMS) based Fenton-like reactions, achieving an exceptional reaction rate constant ( k ) of 0.54 min −1 , which is 2.6 times and 49 times higher than those of Co/TpHz and to Co/TpBD, respectively. Density functional theory (DFT) calculations revealed that modulation of the SCS significantly influences the electronic structure of the Co sites. Notably, the active sites in Co/TpPa exhibited the strongest adsorption energy (–1.60 eV) toward PMS, along with the lowest reaction energy barrier. This work offers valuable insights into the role of the SCS in SACs and opens a new avenue for the rational design of high-performance Fenton-like catalysts.
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.1
Chenyan Lu,Dajie Zou,Ning Zhang,Huye Li,Yanyan Jia,Huan Wang
In this study, the hexane extract of Asters tataricus was used as the carbon source, and ethylenediamine and 4-bromophenylene diamine were selected as dopants to prepare nitrogen and bromine co-doped carbon dots (N,Br-CDs) by the hydrothermal synthesis method. The obtained fluorescent probe has a uniform particle size distribution, good water solubility and high stability, with a fluorescence quantum yield of 48.43%. Under 420 nm excitation conditions, N,Br-CDs exhibited the strongest fluorescence emission at 513 nm, indicating that the sensing system was in the “ON” state. Subsequently, TA was introduced as a quencher to induce static quenching of the N,Br-CDs system, significantly weakening the fluorescence intensity and switching the sensing system from “ON” to “OFF”. Finally, after EM was introduced into the N,Br-CDs/TA system, EM preferentially formed a complex with TA and weakened its quenching effect on the quantum dots, thereby achieving fluorescence recovery and returning the sensing system from the “OFF” state to the “ON” state. Based on the above mechanism, an “ON-OFF-ON” fluorescence sensing system with N,Br-CDs as the luminescent substrate was constructed for the sensitive detection of TA and EM. The results showed that the system exhibited good linear response to TA, with the linear ranges being 1.50–22.94 μM and 34.88–348.42 μM, respectively, and the limits of detection being 0.2168 μM and 2.1797 μM, respectively (LOD, S/N = 3). The linear range for EM was 1.93–377.08 μM, with a detection limit of 0.6693 μM. Furthermore, the sensor system was capable of quantitatively determining TA and EM in human serum, Huangshui River water, and milk matrices, demonstrating its potential for broad application in environmental monitoring and bioanalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 21.1
Yuqing Feng,Hongxia Liu,Yongxing Shang,Yingsen Fang,Shumei Gao,Ping Sun,Bitao Xiong,Hui Wang,Hui Liu,Mingbao Feng
Single-atom catalysts (SACs) are an effective strategy for maximizing the efficiency and reducing the costs of advanced oxidation processes (AOPs). Herein, a novel SAC with Fe−N 3 C sites was synthesized for emerging periodate (PI)-based AOPs. The optimized catalyst demonstrates superior performance, achieving 100 % removal of diclofenac (DCF) within 20 min via predominant singlet oxygen ( 1 O 2 ). Compared to the Fe−N 4 configuration, the Fe−N 3 C site enables an unprecedented 152.9-fold increase in the pollutant degradation rate, surpassing most reported catalysts. Density functional theory (DFT) calculations reveal that the Fe−N 3 C sites reduce the oxophilicity of the Fe centers, thereby lowering the energy barrier for 1 O 2 desorption and promoting its preferential generation. The DCF degradation pathway was further elucidated by Fukui constants. Furthermore, the Fe−N 3 C/PI system exhibits excellent stability with negligible leaching of Fe ions and strong resistance to common wastewater components. This work provides new insights into the design of efficient SACs and the construction of PI-based AOPs for water decontamination.
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ChemistrySelect
·
2026
·Vol. 11
·期 1
·e05099
·
IF 2
Rui Wang,Dayu Sun,Chenyu Zheng,Jingyi Gan,Ruiping Wei,Wei Xu,Guomin Xiao,Lijing Gao
Lignin, a crucial natural aromatic polymer, presents a pivotal challenge in achieving high-value utilization of biomass through depolymerization into aromatic compounds. To address the limitations of conventional lignin depolymerization processes, including harsh reaction conditions, poor catalyst recovery, and low product selectivity, this study establishes a green oxidative system based on the synergistic interaction between the magnetically separable spinel-structured MgFe 2 O 4 and hydrogen peroxide (H 2 O 2 ), systematically investigating its catalytic performance for enzymatic hydrolysis lignin (EHL) depolymerization. The MgFe 2 O 4 was synthesized via a solvothermal method, demonstrating excellent catalytic activity. Under optimized reaction conditions (10% H 2 O 2 , 0.075 g catalyst, 80°C, 4 h), the lignin oil yield reached 51.30%, with significantly enhanced aromatic monomer selectivity of 134.2 mg/g. Moreover, the products exhibited a notable reduction in molecular weight along with increased phenolic hydroxyl and carboxyl group contents. Based on the Fenton-like mechanism involving the dynamic Fe 3+ /Fe 2+ redox cycle, a regulation pathway of reactive oxygen species was proposed. Additionally, the catalyst exhibited exceptional stability with 88.9% retention of initial activity after four magnetic separation cycles. This work proposes a green catalytic strategy integrating high activity, selectivity, and recyclability for efficient lignin depolymerization, providing critical insights for advancing biomass refining technologies. Graphical This work presents a sustainable MgFe 2 O 4 /H 2 O 2 catalytic system for lignin valorization. The magnetically recoverable MgFe 2 O 4 enables efficient oxidative depolymerization of enzymatic hydrolysis lignin (EHL) under mild conditions, achieving 134.2 mg/g aromatic monomers. A Fenton-like mechanism drives selective β-O-4 bond cleavage, while catalyst stability (> 88% activity after four cycles) highlights its potential for green biorefineries.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2026
·Vol. 123
·期 2
·e2521306123
·
IF 9.1
Yuxi Zhao,Man Tong,Li Tian,Genming Luo,Ping Li,Haijun Song,Zhong-qiang Chen,Shucheng Xie,Andreas Kappler,Songhu Yuan
The great phytoplanktonic shift from green to red plastid lineage dominance in the early Mesozoic marks a primary producer revolution in marine ecosystems, facilitating the rise of modern ecosystems and impacting global carbon cycling and energy flows. The causes driving this evolutionary transition have been attributed to the changes in essential nutrients and the environmental crises of the Permian–Triassic mass extinction. Nonetheless, the underlying mechanisms driving this transition remain poorly understood. Here, we integrated culture experiments, molecular and physiological analyses, big data analysis, and phylogenomic dating analyses to uncover how environmental stresses influence algal physiology, thereby altering their evolutionary trajectories. We find that environmental and endogenous reactive oxygen species (ROS) collaboratively shape phytoplanktonic responses. The structural characteristics of red lineage phytoplankton enhance resistance to environmental ROS, facilitating physiological strategies that minimize endogenous ROS accumulation, thereby driving more adaptive evolutionary trajectories under environmental stresses in the early Mesozoic. The alignment of the turnover in diversification dynamics between the two lineages with paleoenvironmental shifts that triggered increased ROS production supports the role of ROS in driving this evolutionary transition. Our findings highlight ROS as a key underlying factor driving phytoplankton evolution, providing predictive insights into major biota–environment coevolutions throughout Earth’s history.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Zhimo Fang,Zhou Zhou,Xiaomeng Li,Dongyang Li,Bin Hu,Haoyu Wang,Lin Zhang,Qin Dai,Kai Li,Yao Kong,Shiguan Yang,Qiang Lu
Superexchange-mediated dual-acceptor sites enable spatial charge separation. • Synergistic single-atom and vacancy engineering creates multifunctional sites. • Cu SA -TO-O V delivered excellent corresponding turnover frequencies of 177.52 h −1 . • The photo-Fenton system exhibited wide pH adaptability and anti-interference. Synchronously and efficiently utilizing photogenerated electrons and holes remains a significant challenge in Fenton-like reaction. Herein, the Cu single-atom (Cu SA ) and oxygen vacancy (O V ) co-modified TiO 2 nanoflake-like catalyst is successfully synthesized. O V modulate the electronic coupling interaction, which is proposed to trigger superexchange -mediated electron transfer from Cu 3 d x 2 − y 2 to Ti 3 d xy via O 2 p y orbitals. Specifically, Cu SA serves as the hole-accepting site for 1 O 2 generation, while O V and Ti 3+ functions as the electron-accepting site for •OH production and contaminant adsorption. The substrate enrichment effect and the free radical/non-radical coupling interaction significantly enhances photo-Fenton catalytic performance, achieving superior sulfanilamide removal efficiency across a broad pH range (3–11) and a high turnover frequency of of 177.52 h −1 . This work not only highlights the potential of active site engineering in designing photo-Fenton catalysts but also advances the development of efficient and sustainable water purification solutions.
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