JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Xin-Yu Chang,Hong-Wei Li,Yuqing Wu
The composites of H 2 N-ZIF-8 supported gold nanoclusters (AuNCs@H 2 N-ZIF-8) were prepared by UV-induced photochemical reduction method in the methanol–water solution. The photochemical reaction was attributed to the generation of free radical as. CH 2 ·–OH, which reduced Au(III) to Au(0) and produced monodisperse AuNCs (<2.5 nm) in the mesoporous of H 2 N-ZIF-8. The generated AuNCs@H 2 N-ZIF-8 show oxidase-like properties to catalyze the oxidation of TMB, ABTS and OPD under mild conditions. Besides, the mechanism study by EPR shows that the composites can promote oxygen to generate singlet oxygen ( 1 O 2 ) and superoxide radicals ( ·O 2 - ), endowing it excellent catalytic activity of oxidation. Further studies revealed that the large number of exposed small AuNCs in the mesoporous pores of H 2 N-ZIF-8 and the highly active 211 crystalline facets formed at the edges contribute to the ROS generation intrinsically. Therefore, the present study demonstrates the significance of photochemical reduction method to prepare highly efficient oxidase-like materials, opening up a new avenue to construct noble metal materials as ultra-small nanozyme.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jing Wang,Wenlei Wang,Yao Deng,Ting Yang,Zhen Zhang,Hui Wang,Yiqiang Wu
Chiral nanomaterials typically exhibit special optical activities, such as optical rotation and chiral photomechanics, and have enormous potential for applications in molecular chiral photocatalysis and other fields. In this work, cellulose nanocrystals (CNCs) were obtained from renewable and affordable bamboo resources through the steps of delignification, hemicellulose removal and acid digestion. Meanwhile, ZIF-8 materials with truncated rhombic dodecahedral structure were obtained by liquid-phase synthesis from Zn 2+ coordinated with 2-methylimidazole (2-MiM). And then, the topologically chiral CNCs@ZIF-8 3D network was successfully constructed by using CNCs as a bridge to graft with ZIF-8 through the formation of Zn–N–S and Zn–O–S bonds. The photoreduction yield of CO 2 to CO by CNCs@ZIF-8 (α = +21.290) with topological chirality was 301.16 μmol −1 ·g −1 , which was 9.43 times that of ZIF-8 (α = 0.000). Density functional theory (DFT) calculations confirm that Zn–O–S with a larger bond angle (118.0°) was conducive to charge accumulation. Photoelectric test results show that CNCs can improve the electron transport ability and reduce the rate of photogenerated electron-hole complexation in ZIF-8. This work elucidated the mechanism of chiral auxiliaries in photocatalytic reduction of CO 2 and provided a new strategy for photocatalytic reduction of CO 2 .
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ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Wenling Wu,Xuan Zhang,Anding Shao,Gang Zhen,Yang Cheng,Xiangfei Wang,Jianfeng Zhu,Hongjie Luo
The corrosion of ancient bronze relics and protection measures after excavation are of great importance to the study of historical and cultural heritage. At present, the bionic superhydrophobic surface anticorrosive coating is one of the main anticorrosive measures of bronze cultural relics. It aims to construct a barrier to prevent the contact between corrosive media and bronze to reduce the invasion of corrosive media. However, due to structural defects such as micropores in a single organic coating, corrosive media (O2, Cl–, and H2O) can penetrate the coating to the metal matrix. Nanomaterials such as MXenes and metal–organic frameworks (MOFs) can fill structural defects such as microholes and microcracks of the coating, thereby improving the density of the coating. Therefore, to improve the performance of organic waterborne polyurethane (WPU) coatings with good chemical protection, nanomaterial ZIF-8/Ti3C2Tx was introduced based on the organic–inorganic hybrid theory. Finally, the coating was modified by 1H,1H,2H,2H-perfluorodecyltriethoxysilane, and the organic–inorganic composite coating was prepared. Characterizations of the composite coating were performed via Fourier transform infrared spectroscopy, X-ray diffraction, Brunauer–Emmett–Teller method, field-emission scanning electron microscopy/energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. Colorimetric measurements and reversibility experiments of the coating were also evidenced. According to the electrochemical impedance spectroscopy assessments, the |Z|0.01 Hz value of the F-WPU@ZIF-8/Ti3C2Tx composite coating in a 3.5 wt % NaCl solution, which was higher compared to other composite coatings. Moreover, the icorr value of the F-WPU@ZIF-8/Ti3C2Tx (3.344 × 10–6 A cm–2) composite coating is reduced by 2 orders of magnitude compared with F-WPU@ZIF-8 and F-WPU@Ti3C2Tx coatings. As a result, this organic–inorganic F-WPU@ZIF-8/Ti3C2Tx composite coating has good anticorrosion properties to bronze without causing an obvious color difference change and has potential application prospects in various metal material fields.
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Molecular Catalysis
·
2024
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IF 3.9
Pushuang Xing,Cong Li,Yixin Chen,Rong-Lan Zhang
PMoV 2 was encapsulated in four MOFs (MIL-101, HKUST-1, UiO-67, ZIF-8) with different cavity sizes and window sizes using a hydrothermal synthesis method. Then, a layer of mesoporous silica was coated on the surface of the MOFs to obtain four designed three-layer encapsulated catalysts 30%PMoV 2 @MOF@mSiO 2 . The physicochemical properties of the catalysts were characterized through various characterization methods, and the influence of different MOF window sizes of the four catalysts on the removal rate of four thiophene sulfides was investigated. The optimal reaction conditions were also explored for the optimal catalyst. The results indicate that under simulated fuel of 2400 ppm, 30%PMoV 2 @UiO-67@mSiO 2 owns the highest catalytic activity. Under optimal conditions, the total removal rate of four thiophene compounds was 91.52 %, and after ten cycles, the efficiency could still reach 86.24 %. This is attributed to the sufficient cavity size of UiO-67, which provides assurance for the loading of PMoV 2 and the large window size, making it possible for the smooth reaction between sulfides and PMoV 2 .
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 27
·12387-12398
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IF 2.7
Yafeng Jin,Fangming Han,Tao Wang,Haofu Shi,Xiaobo Li,Li Yang,Na Chen,Kaifeng Yang,Xinyue Song,Guangri Xu
Developing a facile and effective assay method is crucial due to the potential harm of metronidazole (MNZ) antibiotics to both human health and the environment. Herein, snowflake-shaped poly(3-thiophenemalonic acid, 3-TPA) combined with a carbonized core–shell-type ZIF-8@ZIF-67 (C-ZIF-8@ZIF-67) hollow polyhedra modified glassy carbon electrode (GCE), denoted as C-ZIF-8@ZIF-67/P3TPA/GCE, was fabricated by electropolymerization followed by the electrodeposition strategy. The resulting sensor demonstrates a significant electrocatalysis effect for the reduction reaction of MNZ, exhibiting a broad linear range (0.1–20, 20–800 μM) with a low limit of detection (LOD, 3S/N) of 0.024 μM. Furthermore, it has been successfully applied to determine MNZ in tablets and lake water. A synergistic effect between P3TPA and C-ZIF-8@ZIF-67 is elucidated through density functional theory (DFT) calculations. Consequently, this research introduces a sensitive and effective method for monitoring MNZ in real samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Zhiqiang Guo,Juanjuan Meng,Xinxin Li,Xinlong Wang,Yuan Li,Liangliang Hu
Layered double hydroxides (LDHs), despite their unique layered structure advantageous for removing high-molecular-weight antibiotics, suffer from limitations such as small specific surface area, uncontrollable morphology, and irregular spatial structure compared to metal–organic frameworks (MOFs). Therefore, in this study, ZIF-8 was used as a template to prepare LDHs with a hollow mesoporous structure (ZNF-HS), merging the benefits of both materials. ZNF-HS was then stably incorporated into sodium carboxymethylcellulose aerogels, resulting in ZNF-HS@CMC composites that facilitated easy solid–liquid separation and were effective in removing tetracycline (TC) and ciprofloxacin (CIP) from aqueous solution. Characterization of ZNF-HS@CMC was conducted using SEM, TEM, XRD, FTIR, XPS, BET, and TGA. ZNF-HS@CMC exhibited a specific surface area of 248.753 m 2 ·g −1 and a pore volume of 0.568 cm 3 ·g −1 , surpassing traditional LDHs. The removal of TC and CIP by ZNF-HS@CMC followed the pseudo-second-order kinetic and Langmuir models, with maximum sorption capacities of 513.772 and 442.515 mg·g −1 , respectively. pH significantly influenced the removal efficiencies, while NaNO 3 concentration up to 0.25 mol·L −1 had negligible impact, maintaining removal efficiencies above 90 %. After five sorption–desorption cycles, the removal efficiencies remained above 80 %. The removal of TC and CIP by ZNF-HS@CMC was primarily achieved through surface complexation, hydrogen bonding, and π-π interactions, with electrostatic interactions also contributing. Overall, ZNF-HS@CMC exhibits the advantages of easy recycling, good reusability, strong resistance to salt interference, and high sorption capacity, making it promising for practical applications in the efficient removal of antibiotics from water.
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RENEWABLE ENERGY
·
2024
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IF 9
Wenli Zhang,Jifei Liu,Hongwei Gu,Cheng Pan,Yifei Long,Qunpeng Cheng,Guozhi Fan
The metal-organic framework materials ZIF-8 and UiO-66-NH 2 , synthesized by hydrothermal methods, were characterized in detail and combined to catalyze the transfer hydrogenation of 5-hydroxymethylfurfural (5-HMF) to 2,5-di(hydroxymethyl)furan (2,5-DHMF) using isopropanol as the hydrogen source. The ZIF-8/UiO-66-NH 2 catalyst mixture exhibited abundant Lewis acid-base sites and a hierarchical multiporous structure with a large specific surface area (564.0 m 2 /g). The conversion of 5-HMF reached 98.2 %, and the selectivity and yield of 2,5-DHMF were 96.2 % and 94.5 %, respectively. The recycling performance of ZIF-8/UiO-66-NH 2 was also investigated, and the conversion of 5-HMF and selectivity of 2,5-DHMF significantly decreased to 78.4 % and 79.1 % in the second run, respectively. The loss of −NH 2 groups was found to be the main reason for the decrease in activity. However, the catalytic activity of the recovered catalyst can be almost completely restored by the addition of a small amount of fresh UiO-66-NH 2 and ZIF-8, and the conversion of 5-HMF and selectivity of 2,5-DHMF were increased to 89.4 % and 95.5 %, respectively. In the proposed reaction mechanism, Lewis acid-base sites play important roles and exhibit a synergistic catalytic effect in the selective conversion of 5-HMF to 2,5-DHMF.
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ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Junchun Guo,Li Xu,Lian Ou,Jinmi Zhang,Jianlong Li,Hongmei Huang,Xiaoli Xiong
As a persistent industrial pollutant, the accurate detection of nitrobenzene (NB) holds critical importance in environmental monitoring and health risk mitigation. Recently, the strategy of using metal-organic frameworks (MOFs) as self-sacrificial precursors/templates to design electrocatalysts with unique structures and excellent electrochemical sensing properties has been regarded as a promising approach. Herein, using ZIF-8 supported on hollow carbon spheres as a self-sacrificing model, a hierarchical electrocatalyst (N HCS@HSC) with a dual - hollow carbon nanostructure composed of N-doped hollow carbon spheres (N HCS) and fishnet-like nanonesh (HSC) was prepared. Benefiting from the interconnected hollow channels in the carbon nanomesh, accelerated electron transfer is achieved, with N-doping further engineering the catalyst's local charge density to optimize active sites. The micro-mesoporous ZIF-8-derived carbon is not only beneficial to the selective recognition of NB, but also enhances the electrically conductive of the catalyst and greatly alleviates the aggregation of active sites. The N HCS@HSC sensing platform demonstrates a broad dynamic response range (0.3–254 μM) with a low detection threshold (0.042 μM) toward NB, coupled with remarkable selectivity and long-term operational stability, which has important implications for human health and environmental safety.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yixin Pan,Bo Sun,Yingying Zhou,Jian Jiao,Liping Deng,Xiaowu Dong
This study reported a Ni 0 @ZIF-8 nanocomposite synthesized via co-precipitation that synergistically integrated the high adsorption capacity of ZIF-8 with the redox activity of zero-valent nickel (Ni 0 ) for efficient uranium(VI) extraction. The composite with an optimized 1:1 ZIF-8:Ni 0 molar ratio achieved an exceptional adsorption capacity of 830.5 mg/g. Kinetic and thermodynamic analyses confirmed chemisorption-dominated monolayer adsorption following pseudo-second-order kinetics (R 2 > 0.999) and spontaneous endothermic behavior. Mechanistic investigations through spectroscopy and density functional theory (DFT) calculations revealed a dual-function mechanism that ZIF-8 facilitated U(VI) capture through electrostatic/coordination interactions, while Ni 0 mediated partial reduction of U(VI) to U(IV) via electron transfer, enhancing immobilization stability. Notably, only Pb 2+ , Cu 2+ , Cr 6+ , and organic ligands inhibited adsorption through redox competition and solution complexation. Comparative studies demonstrated minimal matrix interference-deionized water versus seawater systems exhibit merely 4.7 % deviation in adsorption efficiency at trace U(VI) concentrations (0.1–0.6 mg/L). Critically, direct uranium extraction from unprocessed natural seawater (ambient U: 4.27 μg/L) with only pH adjustment (5.0) achieves 86.02 % efficiency at ultra-low adsorbent dosage (0.001 g/L), yielding residual uranium concentrations of 0.597 ± 0.04 μg/L. By harmonizing adsorption and redox pathways, Ni 0 @ZIF-8 overcome limitations of conventional materials, establishing itself as a paradigm-shifting solution for uranium remediation in complex ionic matrices and real marine environments.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
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IF 9
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Yixuan Wang,Xingxiang Zhang,Xuhuan Yan,Na Han
Polyphenylene sulfide (PPS) membrane materials have attracted significant attention for separating oily wastewater due to their remarkable separation precision and permeation capability. Nevertheless, the inherent hydrophobic characteristics result in a single wetting property, which restricts their broad applicability in treating diverse types of oily wastewater. In this study, the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes exhibit outstanding under-liquid dual superlyophobicity, which were formed via constructing a composite coating containing polyphenol-polycation and calcium alginate (CaAlg) hydrogel, and assembling ZIF-8 nanocrystals with suitable surface chemistry. Through the solvent pre-wetting approach, the surface wettability of the PPS composite membranes can be flexibly transitioned between under-water superoleophobicity and under-oil superhydrophobicity, thus realizing on-demand separation of oily wastewater. It is noteworthy that the treatment efficiency of the PPS/TA-PEI/CaAlg/ZIF-8 composite membranes for the various oil-water mixtures (surfactant-free) and emulsions (stabilized by surfactants) attained greater than 98.1%. Meanwhile, the rapid transport capability of diverse types of oil-water emulsions can also be exhibited, with a permeance of 1652.4 L m -2 h -1 bar -1 for water-in-oil (W/O) emulsions and 2087.5 L m -2 h -1 bar -1 for oil-in-water (O/W) emulsions. In addition, the PPS composite membranes demonstrated outstanding anti-fouling capacity, recyclability, and switchable separation capacity. This work extended the utilization of the PPS membrane material in the controllable treatment of oily wastewater.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Yiwen Li,Shikuan Xu,Yangyang Zhang,Rui Du,Rong Li,Yanjun Xing
MimDES-ZIF-8 with rich active sites as positive charges and metal coordination sites were prepared based on imidazole based deep eutectic solvent (MimDES) using interface permeation method. 2-Methylimidazole (2-Mim) simultaneously acted as a hydrogen bond acceptor (HBA) in MimDES (hydrogen donner was 1,6-hexanediol) and an organic ligand in MimDES-ZIF-8, affecting the coordination of ZIF-8 during permeation. Four different zinc salt solutions (ZnCl 2 , Zn(NO 3 ) 2 ·6H 2 O, Zn(OAc) 2 ·2H 2 O, ZnSO 4 ·7H 2 O) were permeated into MimDES to obtain MimDES-ZIF-8 with different morphologies. All MimDES-ZIF-8 had higher Zn/N ration (>0.25), specific surface area and surface positive charges. The dye adsorption results indicated that MimDES-ZIF-8 showed high adsorption efficiencies for acid fuchsin (all exceeded 97.75 % under pH 7.5) and a fast adsorption rate (exceeding 93 % in 5 min and reaching equilibrium in 60 min). Among MimDES-ZIF-8, the adsorption capacity of ZIF-8-C was 4845.3 mg/g. After five cycles of adsorption, the AF removal efficiency of ZIF-8-C remained over 93.23 %. Moreover, ZIF-8-C also had good adsorption capacity for anionic dyes CR, cationic dyes MB and BB. The adsorption process aligned well with both the Langmuir model and the pseudo-second-order kinetic model. Based on FTIR, XPS, and electrostatic potential calculation, the adsorption mechanism was elucidated.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Ya-Ting Qin,Hui Peng,Xi-Wen He,Wen-You Li,Yu-Kui Zhang
A multifunctional diagnosis and treatment integration platform is crucial in cancer treatments. Here, we show that by integrating Gd-doped silicon nanoparticles (Si–Gd NPs), chlorine e6 (Ce6), doxorubicin (DOX), zeolitic imidazolate framework-8 (ZIF-8), poly(2-(diethylamino)ethyl methacrylate) polymers (HOOC-PDMAEMA-SH), and folic acid–poly(ethylene glycol)–maleimide (MaL–PEG–FA) into one single nanoplatform by a self-assembly method, novel multifunctional MOFs (named FZIF-8/DOX–PD–FA) are synthesized with great biocompatibility and tumor targeting as well as pH responsiveness and no drug leakage for drug delivery. In the design, Si–Gd NPs and Ce6 embedded in the nanocomposites are used for magnetic resonance and fluorescence dual-modal imaging, respectively. DOX loaded by the FZIF-8/DOX–PD–FA porous structure is used for chemotherapy, while Ce6 is excited by near-infrared radiation (NIR) for photodynamic therapy. In addition, the pH-responsive ability of HOOC-PDMAEMA-SH to effectively prevent drug leakage is demonstrated by drug release studies in vitro. From the results of confocal microscopy imaging in vitro and fluorescence/magnetic resonance imaging in vivo, FZIF-8/DOX–PD–FA showed a targeting effect on MCF-7 cancer cells. More importantly, the results of treatment experiments on tumor-bearing mice showed that the tumor volume of the FZIF-8/DOX–PD–FA + NIR group is decreased the most compared to the original volume. Owing to the unique dual-modal imaging capability and excellent chemo-/photodynamic combinational cancer therapy effect, the present hybrid nanocarrier provides a new research platform for a new generation of theranostic nanoparticles.
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DOI
PubMed
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