APPLIED SURFACE SCIENCE
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2024
·
IF 6.3
Bingbing Cui,Guodong Fu
Given that heterojunction engineering is an effective method for improving the separation efficiency of photoexcited electrons in WO 3 -based photochromic systems, a series of solid-state photochromic Zr/Ti-MOF@WO 3 heterojunctions prepared via a facile hydrothermal strategy, where Zr/Ti-MOF with photosensitivity and chemical stability was selected as template to load WO 3 . Zr/Ti-MOF@WO 3 heterojunctions were verified as nanoparticles filled with thin layer structure and WO 3 was diffused into the Zr/Ti-MOF planar. The appropriate conductive band energies facilitate the transport of photostimulated electrons from Zr/Ti-MOF to WO 3 , resulting in a fast photresponse in color changes (it only takes 1 s). In addition, a carrier for information storage and data dynamic encryption was developed on the basis of the photochromic Zr/Ti-MOF@WO 3 heterojunctions. This work presents a promising way to improve the electron/holes separation efficiency by constructing unique heterojunctions and further explore novel WO 3 -based photochromic systems and broaden their applications in rewritable media and data security.
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SURFACE & COATINGS TECHNOLOGY
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2024
·
IF 5.3
Jiangtao Yu,Yan Lou,Zhaoyi Wang,Guijian Huang
Self-assembled monolayers (SAMs) technology is considered a potential surface modification technique for addressing challenges in micro/nanostructure fabrication. Bulk metallic glasses (BMGs) are ideal materials for micro/nanostructure moulds. In this study, the surface of Zr-based bulk metallic glasses (Zr-based BMGs) was modified using phosphonic acid SAMs. The findings indicate that phosphonic acid SAMs can effectively reduce the surface free energy of Zr-based BMGs, successfully converting its surface from hydrophilic to hydrophobic and significantly reducing its friction coefficient by up to 90.0 %. Moreover, compared to traditional crystalline Zr-3 alloy, SAMs technology provides significantly better modification effects on amorphous Zr-based BMG surfaces. Experimental results show that among the three different SAMs, the packing density is highest for the mixed hexylphosphonic acid–dodecylphosphonic acid (HPA–DDPA) SAMs, followed by pure dodecylphosphonic acid (DDPA) SAMs, with pure hexylphosphonic acid (HPA) SAMs showing the lowest packing density. The water contact angle for HPA–DDPA SAMs reaches 101.4°, representing a 68.7 % increase compared to the bare plate. Additionally, phosphonic acid SAMs can significantly reduce the friction coefficient of Zr-based BMG surfaces, effectively suppressing oxidative wear and abrasive wear , thereby improving surface wear resistance. The packing density of phosphonic acid SAMs is the primary factor influencing surface wettability and frictional performance, with both wettability and frictional performance increasing monotonically as packing density increases. This is attributed to shear forces and van der Waals forces at the interface. Under specific loads, HPA–DDPA SAMs exhibit excellent lubrication and wear resistance, attributed to the elastic response and compliance of the SAMs. In conclusion, this paper successfully prepares various phosphonic acid SAMs on Zr-based BMGs surfaces and provides a detailed elucidation of the enhancement mechanisms in hydrophobicity and wear resistance through the study of SAMs molecular packing density.
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Catalysts
·
2024
·Vol. 14
·期 12
·924
·
IF 3.8
Yu Yue,Guozhi Zhu,Min Liu,Yue Zhu,Weilong Ji,Xiaoqin Si,Tianliang Lu
As an important biomass resource, γ-valerolactone (GVL) shows considerable potential for applications in biofuel production, organic synthesis, polymer, and food industries. Herein, an effective method was presented for synthesizing GVL through the catalytic transfer hydrogenation (CTH) of ethyl levulinate (EL) under mild conditions. Using isopropanol as a hydrogen donor, a 100% conversion of ethyl levulinate and an 88.7% yield of GVL were achieved over 2%Zr-Beta-7d catalyst at 110 °C for 8 h. The acidic sites of synthesized Zr-Beta via hydrothermal methods easily adjusted and offered high catalytic activity and selectivity. The Lewis (L) acid sites on the zeolite serve as the active centers for the conversion of EL. Characterization results indicate that the amounts of L acid sites on Zr-Beta increased with the Zr content and crystallization time rose, thus enhancing the selectivity for GVL. Additionally, the influences of catalyst dosage, reaction temperature, and time on catalytic performance are studied, as well as calculations of kinetic parameters such as reaction rate constants and activation energies. The 2%Zr-Beta-7d catalyst retains its high performance after five cycles. The current research may present an efficient approach for the conversion of EL to GVL under mild conditions.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Juan Chen,Tingting Guo,Hongyi Gao,Han Meng,Zhixin Zhang,Jie Li,Zhili Song,Xingyu Pei,Supakorn Boonyuen,Xiaowei Zhang,Yu Jiang,Jinzhang Tao
The application of mixed-linker strategies in the synthesis of metal-organic frameworks (MOFs) has garnered considerable interest owing to their potential as fluorescent sensors, attributed to their facile synthesis and incorporation of diverse functional ligands. In this study, we designed and synthesized a novel fluorescent Zr-based MOFs, denoted as MOF-808-NH 2 , through the post-synthetic modification of 2-amino terephthalic acid (BDC-NH 2 ) on coordinatively unsaturated Zr sites, thereby preserving the structural stability of the parent framework. The MOFs exhibited exceptional turn-on fluorescence in aqueous solutions containing fluoride ions (F − ). The interaction between the-NH 2 groups on MOF-808-NH 2 and F − facilitated the formation of hydrogen bonds, significantly enhancing the fluorescence emission intensity of BDC-NH 2 at 450 nm and inducing a blue shift in the fluorescence emission peak, enabling the specific recognition of F − even in the presence of various anionic interferences. Notably, MOF-808-NH 2 demonstrates an ultrafast response time (within 30 s), a high detection sensitivity with a limit of detection of 1.56 μM, and remarkable selectivity and anti-interference properties with pronounced fluorescence emission against a dark background. Furthermore, MOF-808-NH 2 retained outstanding thermal, mechanical, and chemical stabilities, underscoring its potential for practical applications in selective F − detection.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Fuhua Wei,Jie Gong,Qinhui Ren,Xiang Yu,Yan Wang,Hongliang Chen,Zhao Liang
The Zn/Zr-MOFs were synthesized via microwave-assisted ball milling and subsequently characterized using Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), and scanning electron microscopy (SEM). The thermal stability of the Zn/Zr-MOFs was evaluated through thermogravimetry (TGA). The results demonstrated the exceptional adsorption properties of the Zn/Zr-MOFs towards Lomefloxacin hydrochloride and Levofloxacin hydrochloride. At a concentration of 30 ppm for Lomefloxacin hydrochloride, the addition of 30 mg of Zn/Zr-MOFs material resulted in an adsorption capacity of 179.2 mg•g−1. Similarly, at a concentration of 40 ppm for Levofloxacin hydrochloride, the addition of 30 mg Zn/Zr-MOFs material led to an adsorption capacity of 187.1 mg•g−1. Kinetic analysis revealed that the experimental data aligned well with a pseudo-second order kinetic model. Overall, these findings highlight the significant potential application of Zn/Zr-MOF materials in wastewater treatment.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Linna Han,Zixu Wang,Wanfang Feng,Qing Xia,Yucun Niu,Liyan Liu
Background The enrichment of sugar phosphates (SPx) from complex biological samples was of significant importance for elucidating their roles in physiological and pathological processes. However, the detection of SPx faced numerous challenges due to the high structural similarity among its isomers, its extremely low abundance within cells, the complexity of biological samples, and the inefficiency and cumbersome nature of traditional enrichment methods. Therefore, there was an urgent need to develop an efficient enrichment technique, leveraging the advantages of magnetic separation to achieve precise detection of sugar phosphates in biological samples. Results A novel magnetic material, Fe 3 O 4 @UiO-66-Br, was synthesized for efficient and convenient enrichment of SPx in biological samples. The material exhibited a high specific surface area (225.08 m 2 /g) and strong magnetism (33.61 emu·g −1 ). Only 600 μg of Fe 3 O 4 @UiO-66-Br was required to completely adsorb five types of SPx within 4 min. The adsorption process was pH-tolerant and can be accomplished simply by standing. Kinetic, thermodynamic, and isotherm studies revealed favorable adsorption properties, characterized as spontaneous and endothermic monolayer chemisorption. Mechanistic studies using XPS, FT-IR, and DFT identified multiple interactions, including coordination, hydrogen bonding, and electrostatic interactions. The analytical protocol featured a wide linear range (0.01–10000 ng/mL), low detection limits (0.002–0.01 ng/mL), high precision (RSD<13.21 %), and accuracy (80.05 %–116.41 %). Significance The protocol was successfully applied to real blood samples, demonstrating the potential of magnetic MOFs for SPx adsorption and detection. This novel material and protocol provided an efficient approach for enriching and detecting trace SPx in complex biological matrices, facilitating further studies on their roles in physiological and pathological processes.
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NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Qingtai Chen,Chongchong Wu,Shujie Hu,Lizhi Cui,Yong Zhang,Peng Hu,Zhi Xu,Pei Yu,Miao Yu
Xylanase is a natural and high-efficiency catalyst for the degradation of xylan to reducing sugar. However, the catalytic performance of xylanase is greatly limited by its poor activity and stability at the harsh condition. To overcome this issue, covalent immobilization of xylanase on a magnetic porous MOFs material with core-shell structure, UIO-66-NH2 carrier was applied to improve the catalytic activity and stability of xylanase. Several tools were employed to monitor the preparation and immobilization processes, magnetic properties, and the structural/chemical characteristics of the biocatalyst. 77.9% of the activity for xylanase was retained after immobilization. Moreover, the thermal stability in terms of half-life of the immobilized enzyme was three times higher than that in free form, and which had higher catalytic efficiency for hydrolysis of xylan. Furthermore, the greater temperature and wider pH ranges of the activity stability were achieved for the immobilized xylanase in compared with free one. Notably, the biocatalyst exhibits both excellent storage stability and could be easily separated using a magnet, which is conducive for its reusability. And nearly 70% of its initial activity was retained after seven recycles during the hydrolysis of corn straw. These features indicate that the present immobilization method is promising prospect for the industrial application of enzyme.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Guangyuan Hu,Zhiwei Wang,Changqing Xia,Xinliang Wang,Hongxing He,Zhifeng Nie,Shixing Wang,Weili Li
The recovery of gold from industrial effluents is crucial for environmental conservation, sustainable resource management, and promoting the green development of gold resources. We designed a Zr-based MOF (UKM-78) by incorporating functional organic ligands that resemble amino groups, using MOFs’ inherent sieving effect for ion separation. This novel material exhibited enhanced gold recovery under acidic conditions, with an adsorption capacity three times and an adsorption rate four times higher than those of nonfunctionalized UKM-77. Notably, UKM-78 efficiently captured gold solutions at concentrations as low as 1 ppm and achieved an adsorption rate exceeding 90%, owing to the electrostatic interactions and coordination between its functionalized groups and the synergistic effect of its porous structure. Despite multiple regeneration cycles, UKM-78 retains 99.4% of its adsorption capacity. X-ray photoelectron spectroscopy (XPS), kinetic studies, and thermodynamics collectively demonstrated that Au(III) binding on UKM-78 involved cooperative electrostatic interactions and chemical adsorption through coordination. This study highlights the potential of MOFs for efficient and sustainable recovery of gold from complex waste streams.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Elia Gadallah,Mohamed N. Khalil,Sami Karam,Wael Ali,Jinchao Chen,Xiangmin Xu,Yuan Jing,Fang Li
Designing and fabricating ultrafiltration membranes that possess relatively high permeability while simultaneously maintaining high rejection and improved antifouling properties continues to be a challenge. In this study, we investigated the integration of novel melamine modified Zr-based metal organic frameworks (Zr-MOFs) with nanosheets of graphene oxide (GO) and sulfonated graphene oxide (SGO). These composite materials were synthesized using the solvothermal process and subsequently coated onto the PES membrane surface using the vacuum-assisted dip-coating method. The stability enhancement of the topmost MOF composite layer adhering to the membrane surface is attributed to hydrogen bonding, π-π stacking, and van der Waals interactions. These effects are augmented by the incorporation of polar functional groups such as hydroxyl, carboxyl, sulfonate, and amine groups. The optimized composite membranes incorporating MOFs exhibit enhanced performance, with a permeability of 80.2 L/m 2 h bar, achieving a bovine serum albumin (BSA) rejection of ≥97.8 % and a humic acid (HA) rejection of 98.9 %. Moreover, a flux recovery ratio (FRR) of 89.5 %. To investigate the interactions among the incorporated components, molecular dynamics (MD) simulations were employed in a computational study. The simulations validated hydrogen bond formation and reinforced prior studies, demonstrating the potential of Zr-MOF compositions as effective hydrophilic nanoparticles. The overall results indicate a substantial enhancement in membrane performance and underscore the high potential for practical applications.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Jun Cheng,Lei Qian,Hao Guo,Yuxiang Mao,Yang Shao,Weijuan Yang
In order to solve problems that large molecules of microalgal lipids were difficult to access active sites in micropore structures of traditional metal organic frameworks (MOF), a novel two-dimensional nanosheet catalyst (aminobenzoate-substituted s-triazin-based Zr metal organic frameworks, Zr-TATAB) that exposed more active sites with stronger acidity was synthesized through replacement of trimesate linker in water/acid-resistant Zr-based MOF-808 with 4,4 ́,4 ́ ́- s -triazine-1,3,5-triyltri- p -aminobenzoate (H 3 TATAB) to promote catalytic conversion efficiency of microalgal lipids to biodiesel . The binding energy of Zr increased by 0.2 eV due to electronic shift caused by triazine ring and imine groups in H 3 TATAB ligand, which led to more exposed Zr 4+ active sites in Zr-TATAB catalyst. Due to increase of charge on crystal edges, dissociation of terminal hydroxyl groups was inhibited and Coulomb repulsion was increased. Therefore, Zr-TATAB catalyst possessed higher dispersion to avoid from pore blocking and catalytic deactivation, which enhanced recycling performance of catalyst. Compared with MOF-808, the total number of acid and base sites in Zr-TATAB catalyst increased from 6.0 mmol g −1 to 8.0 mmol g −1 , while strength of acid sites increased with an increased ammonia desorption temperature by 150 °C, which led to an increased catalytic conversion efficiency of microalgal lipids to biodiesel to 98.2%.
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MATERIALS & DESIGN
·
2020
·
IF 6.289
Shuaida Zhu,Xiong Cao,Xiaoqing Cao,Yuqi Feng,Xinbing Lin,Kehua Han,Xiaoxia Li,Peng Deng
In this paper, we studied the effect of M-doped graphitic carbon nitride (M-g-C 3 N 4 , M = Fe, Nd, Ce, Zr, U) as a catalyst for the thermal decomposition of ammonium perchlorate-based molecular perovskite DAP-4. DAP-4 was synthesized by a molecular assembly strategy. G-C 3 N 4 and M-g-C 3 N 4 composite samples were prepared by pyrolytic and co-sintering methods. X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy-energy dispersion X-ray spectrometry, and X-ray photoelectron spectroscopy were used to characterize the morphology, structure, element distribution, and element chemical states of the catalysts. Differential scanning calorimetry was used to elevate the thermal catalytic decomposition effect of g-C 3 N 4 and M-g-C 3 N 4 on DAP-4. The results showed that g-C 3 N 4 and M-g-C 3 N 4 have catalytic activity for the thermal decomposition of DAP-4. Among the tested catalysts, Fe-g-C 3 N 4 had the best catalytic activity for the thermal decomposition of DAP-4, as well as advantages over pure g-C 3 N 4 and other M-g-C 3 N 4 catalysts. Especially, Fe-g-C 3 N 4 reduced the peak temperature of DAP-4 by 75.3 °C, increased heat release by 464 J g −1 , and decreased activation energy by 55.5 kJ mol −1 . Moreover, a possible catalytic mechanism is proposed. This work may offer a new way to promote the application of DAP-4 in the field of solid rocket propellants.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 9
·3337-3347
·
IF 4.39
Panpan Du,Siyuan Li,Xuejiao Wang,Qi Zhu,Ji-Guang Li
Solid-state reaction at 1000 °C produces a series of Li-stuffed Li5+2x(La1−yEuy)3(Ta1−xZrx)2O12 garnet phosphors (x = 0–1, y = 0.05–0.6) that exhibit favorable efficiency and thermal stability for red luminescence under either blue or n-UV light excitation, where the optimal composition was identified to be x = 0.5 and y = 0.4. The concentration quenching of luminescence was determined to occur via electric dipole–dipole interactions. Zr4+ substitution for Ta5+, accompanied by additional Li+ for charge compensation, was found via Rietveld structure refinement and Raman/UV-Vis spectroscopy to profoundly affect the tetrahedral and octahedral occupancies of Li, the symmetry of (La/Eu)O8 dodecahedron, and the bandgap of the host lattice and cation disorder, with which the systematically varying excitation and emission behaviors of Eu3+ were deciphered. The Li6(La0.6Eu0.4)3(Ta0.5Zr0.5)2O12 optimal phosphor showed quantum yields of ∼40 and 48% under 393 and 463 nm excitations, respectively, a fluorescence lifetime of ∼0.66 ms for its main emission at 610 nm, color coordinates of around (0.653, 0.347), and can retain as high as ∼85% of its room-temperature emission intensity at 423 K. The phosphor also exhibited a favorable performance for n-UV excited LED lighting.
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