INORGANIC CHEMISTRY
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2025
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IF 4.7
Xue Luo,Yingying Xue,Leilei Xu,Linshui Lian,Cai-e Wu,Yan Cui,Weixin Zou,Lin Dong,Fei Gao,Mindong Chen
This study presents a systematic investigation into the catalytic oxidation of toluene using metal–organic framework (MOF)-derived porous metal oxide catalysts obtained through controlled pyrolysis. The MOF-derived catalysts (Mn3O4-BTC, CeO2-BTC, Co3O4-BTC) demonstrated remarkable improvements in catalytic activity and stability compared to their commercial counterparts (Mn3O4-c, CeO2-c, Co3O4-c), achieving 90% toluene conversion (T90) at significantly lower temperatures of 240 °C, 241 °C, and 237 °C, respectively. Besides, a comprehensive suite of characterization techniques was employed to elucidate the structure–activity relationships. Specifically, various traditional and in situ characterization techniques, including X-ray diffraction (XRD), N2 physisorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), H2 programmed reduction (H2-TPR), online-tandem thermogravimetry-mass spectrometry (online-tandem TG-MS), and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), were employed to elucidate crystallinity, porosity, morphology analysis, probe surface chemistry, redox properties, real-time tracking of thermal decomposition, and reaction mechanisms during the catalytic oxidation of toluene. It was found that the enhanced catalytic performance could be attributed to the synergistic effects of a high surface area, well-dispersed active sites, and abundant oxygen vacancies. These insights provided fundamental insights into the design and optimization of MOF-derived catalysts for efficient volatile organic compounds (VOCs) abatement in environmental catalysis.
研究领域:
环境催化
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材料科学
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化学工程
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纳米技术
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 8
·648
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IF 3.444
Xiao-Qing Gong,Chuan-Wan Wei,Jia-Kun Xu,Xiao-Juan Wang,Shu-Qin Gao,Ying-Wu Lin
The encapsulated enzyme system by metal-organic frameworks (MOFs) exhibits great potential in biofuel cells, pharmaceuticals, and biocatalysis. However, the catalytic efficiency and the enzymatic activity are severely hampered due to enzyme leaching and deficiency of storage stability. In this study, we immobilized cytochromec(Cytc) into dimethylimidazole-copper (Cu(Im)2) by biomimetic mineralization, and constructed a bioinorganic hybrid material, termed Cytc@Cu(Im)2. Encapsulated Cytcin Cu(Im)2with a nanosheet structure exhibited significantly improved catalytic efficiency, enzymatic activity and kinetic performance. The catalytic efficiency (kcat/Km) for Cytc@Cu(Im)2was ~20-fold higher compared to that of free Cytc. Moreover, the increased activity was not affected by long-term storage. Based on this system, we further constructed a multi-enzyme composite with glucose-oxidase (GOx), termed GOx-Cytc@Cu(Im)2, which exhibited greatly improved enzymatic activity, stability, and excellent selectivity for the detection of low concentrations of glucose. This strategy may provide new insights into the design of enzymes with high activity and stability, as well as the construction of multi-enzyme systems.Keywords:enzymatic immobilization;biomimetic mineralization;multi-enzyme;bioinorganic hybrid material;biosensors
研究领域:
生物技术
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生物化学
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材料科学
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生物催化
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Cuizhu Ye,Xingguang Chen,Junjun Xu,Huiting Xi,Tiantian Wu,Danwen Deng,Jinsheng Zhang,Ganhui Huang
Supported by metal-organic frameworks (MOFs), a new molecular imprinted electrochemical sensor (MIES) taking nano-structure Co 2+ @Fe 3 O 4 as the support point of receptor was developed for highly sensitive detection of GA in this paper. Gold electrode was modified with Co 2+ @Fe 3 O 4 , then Co 2+ @Fe 3 O 4 /Au was soaked and compounded to Fe 3 O 4 @ZIF-67/Au. MIPs film was obtained by potentiostatic polymerization with polypyrrole as monomer and GA as template. SEM, EDS, FTIR, XRD, DPV and EIS characterizations indicate the success of the preparation of the modified electrode . By optimization, the Δ i response of MIP/Fe 3 O 4 @ZIF-67/Au was strengthened from 25.38 μA to 30.84 μA. The MIP/Fe 3 O 4 @ZIF-67/Au sensor showed a superior sensitivity with a lower LOD of 0.297pM (S/N = 3) and a wider linear range of 6–600pM for GA detection, which profits from the combination of high surface area of Co 2+ @Fe 3 O 4 and high porosity of MOFs. Because of the specificity of molecular imprinted polymers (MIPs), our sensor showed advanced selectivity and not affected by similar structure interfering substances. In addition, the stability, reproducibility and real-sample detection were also satisfactory with the recovery rates between 89.5% and 118.4% and the RSD were lower than 5.5%. This sensitive and simple method can be further used to prepare polypyrrole-based MIES suported by MOFs-Co 2+ @Fe 3 O 4 for highly sensitive detection of other small and weight molecules.
研究领域:
分析化学
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电化学
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纳米技术
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材料科学
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产品关联
DOI
高影响因子
BIOMACROMOLECULES
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2023
·
IF 6.2
Qizhen Zheng,Jinhan Sheng,Ji Liu,Xianghan Chen,Ming Wang
Biomineralization of metal–organic frameworks (MOFs) provides a powerful approach for intracellular protein delivery, enabling the study of biological function and therapeutic potential of proteins. However, the potency of this approach is largely challenged by the low efficiency of current strategies for interfacing proteins with MOFs for biomineralization and intracellular delivery. Here, we report a versatile and convenient biomineralization strategy for the rapid encapsulation and enhanced delivery of proteins using MOFs, accelerated by histidine-rich proteins. We demonstrate that the histidine-rich green fluorescent protein (H39GFP) can accelerate the biomineralization of MOFs by promoting the coordination between proteins and metal ions, leading to enhanced protein delivery efficiency up to 15-fold. Moreover, we show that the delivery of H39GFP-fused cytotoxic ribonuclease and bacterial-derived RAS protease can effectively inhibit tumor cell growth. The strategy of promoting the biomineralization of MOFs via histidine-rich proteins for enhanced intracellular delivery could be expanded to other biomacromolecules, advancing their therapeutic potential and the biomedical scope of MOFs.
研究领域:
生物医学工程
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材料科学
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生物化学
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癌症研究
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DOI
PubMed
高影响因子
Materials Today Sustainability
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2023
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IF 7.8
L. Xie,J. Ding,X. Kong,J. Qin,J. Wang
With the development of modern industry and increasing population around the world, the overuse of fossil fuels for energy supply has produced large amounts of CO 2 in the atmosphere. Metal-organic frameworks (MOFs) with tailorable structures and developed porosity have emerged as promising candidates for CO 2 adsorption and separation. However, the synthesis of MOFs by conventional hydrothermal method faces challenges like low crystallization rate and yield, which limits their industrial application for gas adsorption. In this work, a highly efficient microwave (MW)-assisted method was employed for the synthesis of Mg-gallate. The effects of MW conditions on the structure, morphology, and CO 2 adsorption properties of Mg-gallate were systematically investigated. The highest CO 2 adsorption performance (5.37 mmol g −1 at 298 K and 1 bar) was achieved on the Mg-gallate synthesized at 100 °C for 20 min under an MW power of 100 W. The obtained Mg-gallate also exhibited high adsorption selectivity of CO 2 over N 2 (1500) and superior recyclability . Furthermore, the Mg-gallate@PEI composite beads were designed by incorporating the MOF crystals into the polymeric matrix in order to satisfy the industrial application demands. The combined advantages of rapid MW synthesis, excellent adsorption performance, and shaping make the Mg-gallate a promising material for practical CO 2 capture.
研究领域:
化学工程
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材料科学
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环境科学
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能源科学
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DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Zhendong Fu,Feng Guo,Jiahe Qiu,Runchi Zhang,Mingxu Wang,Liping Wang
2-Methylimidazole (MIM) is a classic organic ligand that shows excellent thermal stability and chemical robustness and is widely used in ZIFs. Recently, transformations of MOFs have been realized by using metals or ligands. In this study, we propose a new strategy—adjusting MIM by extending the alkyl chain length —to change the properties of related MOFs. Furthermore, we used copper as the metal core to replace zinc to mimic the active sites of laccases (electron transfer between copper and imidazole ring). As a result, the nanostructures transformed from nanoleaves to nanovesicles, which changed the Cu(II)/Cu(I) ratio from 3.7 to 1.7, as well as the lattice constant (decreased the diffraction angle) and enzyme-like activity (inhibition). In addition, we revealed that superoxidase anions were the main factors responsible for its laccase-like activity. We applied it to detect and discriminate phenolics. Laccase-mimicking activity was best at pH 7.0. When compared to protein laccase, the Cu-MeIm nanozyme had a greater Vmax at the same mass concentration. It was used to identify and distinguish phenolics. In the presence of Cu-MeIm nanozymes, the linear range is 0.1–2 mM and the detection limit of 2,4-DCP is 0.034 mM.
研究领域:
材料科学
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纳米技术
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分析化学
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生物化学
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酶学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Guowen Qian,Yuqian Mao,Yang Shuai,Zhikui Zeng,Shuping Peng,Cijun Shuai
Bioceramics have been extensively used to improve osteogenesis of polymers because of their excellent bone-forming capabilities. However, the inadequate interfacial bonding between ceramics and polymers compromises their mechanical properties . In this study, zeolitic imidazolate framework-8 (ZIF-8) was grown in situ on strontium carbonate (SrCO 3 ) to construct a core–shell SrCO 3 @ZIF-8, which was then added to poly- l -lactic acid (PLLA) to print a SrCO 3 @ZIF-8/PLLA composite scaffold using selective sintering technology. First, ZIF-8 characterized by its multiple organic ligands, forms a robust interface with PLLA. Second, SrCO 3 characterized by its negative zeta potential in solution, exhibits the ability to adsorb positively charged zinc ions . This, in turn, promotes the in situ growth of ZIF-8 on SrCO 3 , eventually achieving perfect bonding between the second phase and the PLLA matrix. Our findings indicated that the composite scaffold exhibited the highest compressive strength (21.93 MPa) and significantly promoted the osteogenic differentiation of mouse mesenchymal stem cells. Moreover, the in vivo results established that the SrCO 3 @ZIF-8/PLLA scaffold significantly accelerated bone regeneration efficiency in rat femur defects. The prepared scaffold, with its favorable mechanical properties and osteogenic activity, shows considerable promise for applications in bone repair.
研究领域:
生物材料
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组织工程
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生物医学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Chemistry
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2022
·
IF 7.613
Y. Wei,R. Zou,Y. Xia,Z. Wang,W. Yang,J. Luo,C. Liu
Water remediation from arsenite [As(III)] is critical to environmental sustainability and human health. Metal-organic frameworks (MOFs) hold great promise for this purpose, while their efficient application requires addressing loading and activation issues. Herein, a new bionanocomposite bead UiO-66/CB was fabricated through simple gelation followed by the freeze-casting method for remediation of As(III)-contaminated water. Highly accessible UiO-66 nanoparticles are uniformly dispersed within the networking pores of the macroporous chitosan bead with high activity retention. Moreover, the fabrication strategy effectively activated the embedded UiO-66 nanoparticles, leading to improving the utilization efficiency of the active sites. The millimeter-sized UiO-66/CB-2.0 performed much more efficiently than the freely dispersed UiO-66 nanoparticles in removing As(III) and even exhibited comparable adsorption to the activated UiO-66 nanoparticles. The maximal sorption capacity of As(III) onto UiO-66/CB-2.0 was larger than 47.9 mg/g (88.6 mg As/g UiO-66) at pH 7. 1 g/L UiO-66/CB-2.0 can reduce As(III) levels (200 μg/L) in groundwater to below 10 μg/L. It could be readily regenerated and reused. Fixed-bed column adsorption by using UiO-66/CB-2.0 could treat ∼1600 bed volumes of As(III)-spiked groundwater to below 10 μg/L. This research provides a versatile route to fabricate high-performance and convenient MOFs biocomposite adsorbents for As(III) remediation.
研究领域:
环境科学
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材料科学
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纳米技术
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水处理
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DOI
高影响因子
BIOMATERIALS
·
2024
·
IF 12.8
Jilong Wang,Chenghu Wu,Yiran Wang,Yecheng Shen,Kerui Wu,Yikai Shi,Tianshou Cao,Shanshan Yuan,Yuting Zhu,Yongheng Bai,Jinhai Huang,Yan Zhang,Junjie Deng
Low-expression antigens, especially neoantigens, pose a significant challenge in immunotherapy for low immunogenicity pancreatic cancer. Increasing the tumor mutation burden is crucial to enhance the expression of tumor antigens and improve tumor immunogenicity. However, the incomplete intervention in DNA stability hampers effective elevation of the tumor mutation burden, thus reducing the probability of neoantigen. To address this issue, we have developed a novel nano-regulator that intervenes in the DNA stability of tumor cells, thereby enhancing tumor mutations. This nano-regulator comprises metal-organic frameworks (MOFs) encapsulating DNA damage agent doxorubicin and DNA damage repair inhibitor siRNA-ATR, enabling simultaneous induction of DNA mutations and inhibition of their repair. Importantly, this regulator, named as MOF DOX&siATR , can modulate the tumor gene expression profile, induce the production of neoantigens of Atp8b1, and enhance the immunogenicity of pancreatic cancer. The characteristics of DNA stability intervention by MOF DOX&siATR hold promise for augmenting the immune response in low immunogenic tumors, making it a potential nanomedicine for the treatment of pancreatic cancer.
研究领域:
癌症生物学
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纳米技术
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免疫疗法
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分子生物学
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 27
·期 8
·2717-2723
·
IF 4.857
Zhuoran Lv,Wujie Dong,Bingquan Jia,Shaoning Zhang,Miao Xie,Wei Zhao,Fuqiang Huang
Graphical Linked by MOFs : Sn 2 O(CN 2 ) with loosely packed crystal structure possesses a metal–organic framework-like porous framework, which mitigates volume expansion and Sn atom aggregation. Sn 2 O(CN 2 ) shows a significantly enhanced lithium storage performance compared to traditional tin oxide. Metal-organic frameworks (MOFs) can become promising electrode materials for advanced lithium-ion batteries (LIBs), because their loosely packed porous structures may mitigate volume expansion and metal atom aggregation, which occur at the respective metal oxides. However, they suffer from poor electrical conductivity and irreversible structural degradation upon charge/discharge processes, which impede their practical utilization. Herein, we investigate MOF-like Sn 2 O(CN 2 ) as a new electrode material. The conductive yet flexible [N=C=N] linkers are tilted between [Sn 4 O] nodes and cross-linked into a porous quasi-layered structure. Such structure offers abundant channels for fast Li-ion transport and tolerance of enormous volume expansion. Notably, anisotropic [N=C=N] 2− arrays hardly migrate so that Sn 0 nanodots are physically separated via robust [N=C=N] 2− framework during discharge, thereby effectively preventing the formation of large Sn islands. Owing to the structural advantage, the Sn 2 O(CN 2 ) electrode exhibits an initial Coulombic efficiency as high as ∼80 %. With the addition of graphite as conductive supporter, the electrode provides 978 mAh g −1 at 1.0 A g −1 even after 300 cycles. Such MOF-like carbodiimides hold potential for the advanced electrodes in LIBs and other battery systems.
研究领域:
材料科学
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能量存储
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电池技术
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产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 13
·4247
·
IF 4.927
Xuan Wang,Qing Chen,Congxiao Lu
Hypoxia-activated prodrugs (HAPs) with selective toxicity in tumor hypoxic microenvironments are a new strategy for tumor treatment with fewer side effects. Nonetheless, the deficiency of tumor tissue enrichment and tumor hypoxia greatly affect the therapeutic effect of HAPs. Herein, we design an active targeted drug delivery system driven by AS1411 aptamer to improve the tumor tissue enrichment of HAPs. The drug delivery system, called[email protected](TA-MOF), uses iron-based MOF as a carrier, surface-modified nucleolin aptamer AS1411, and the internal loaded hypoxia activation prodrug TPZ. Compared with naked MOF, the AS1411-modified MOF showed a better tumor targeting effect both in vitro and in vivo. MOF is driven by GSH to degrade within the tumor, producing Fe2+, and releasing the cargo. This process leads to a high consumption of the tumor protective agent GSH. Then, the Fenton reaction mediated by Fe2+not only consumes the intracellular oxygen but also increases the intracellular production of highly toxic superoxide anions. This enhances the toxicity and therapeutic effect of TPZ. This study provides a new therapeutic strategy for cancer treatment.Keywords:aptamer;MOFs;chemodynamic;chemotherapy;breast cancer
研究领域:
癌症治疗
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药物递送系统
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 1
·169-178
·
IF 8.64
Wei Haisheng,Song Huaxing,Ren Yujing,Yan Xiaorui,Fang Geqian,Wang Wenhua,Ren Wanzhong,Zhu Mingyuan,Lin Jian
Metal-organic frameworks (MOFs) derived Co-based catalysts have received extensive attention in the chemoselective hydrogenation of nitroarenes, while they usually require a lot of solvent during the synthesis and identification of active species. This study explores a solid-phase synthesis strategy to obtain MOF precursors without using any solvent, which is then foamed and pyrolyzed to synthesize the Co@NC-X catalyst. It was found that a nitrogen-doped graphene shell can well encapsulate the Co nanoparticles. The resulting catalyst, which was pyrolyzed at 800°C, exhibited ~100% conversion for the hydrogenation of 3-nitrostyrene and >99% selectivity to 3-vinylaniline. This catalyst also showed excellent stability and good substrate universality for the hydrogenation of extensive substituted nitroarenes. Various characterizations revealed a positive relationship between the catalytic performance and the content of Co—N species tuned by pyrolysis temperature. This work provides a novel and green strategy to design an efficient Co-based catalyst for chemoselective hydrogenation.
研究领域:
催化
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材料科学
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化工
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绿色化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）