COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Chunliang Zhao,Jinghui Wu,Yidi Gao,Jialin Zhou,Leilei Zhang,Chi Wang,Yang Huo,Xianze Wang,Mingxin Huo
The rapid increase in PLA product consumption has led to significant environmental challenges. To address this issue, this study focuses on developing efficient catalysts to accelerate PLA alcoholysis, aiming to enhance degradation efficiency. A novel composite catalyst, SiWMn Ⅲ @MIL-125(Ti), was synthesized by encapsulating Keggin-type polyoxometalate (POM) in the octahedral cavities of MOF(MIL-125(Ti)). The compound was comprehensively characterized, while density functional theory (DFT) calculations further confirmed the potential localization of POM within the MOF. The catalyst exhibited excellent efficiency in the alcoholysis of polylactic acid (PLA) using ethylene glycol (EG) under optimum conditions (1 wt% catalyst, 160 °C, 30 min, EG/PLA molar ratio = 4:1, 18 % POM loading), achieving high PLA conversion. The liquid products were systematically analyzed, proposing their oligomeric structures. Notably, this heterogeneous catalyst could be easily retained by filtration and could be reused for more than 10 cycles without significant activity loss. Combined with DFT simulations, a reasonable catalytic mechanism was elucidated, highlighting the synergistic role of POM@MOF in facilitating alcoholysis of PLA. This work not only provides insights into the design of efficient MOF-based catalysts for polymer degradation but also suggests the potential applicability of POM@MOF systems in other depolymerization processes.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2013
·Vol. 2014
·期 2
·345-351
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IF 3.12
Mei-Lin Wei,Jing-Jing Sun,Xian-Ying Duan
Graphical A 3D metal–Schiff-base–POM-MOF has been constructed by combining in situ two traditional building blocks, a metal–Schiff-base and POM-MOF, and its structure was determined by single-crystal X-ray diffraction. Due to the bonding of H 2 O to otherwise open coordination sites on Cu 2+ ions, it shows good proton conductivities of 10 –5 –10 –4 S cm –1 in the temperature range of 25–100 °C under 98 % RH. A metal–Schiff-base–POM-MOF, {[Cu 3 (L) 2 (H 2 O) 4 ] [Cu(dmf) 4 (SiW 12 O 40 )] · 9H 2 O} n {L = N , N′ -bis[(2-hydroxy-3-methoxyphenyl)methylidene]hydrazine hydrate}, has been synthesized in situ from [SiW 12 O 40 ] 4– , Cu 2+ and L in an H 2 O/dmf/CH 3 OH/CH 3 CN mixture at room temperature, and the product was characterized by elemental analysis, IR spectroscopy and single-crystal X-ray diffraction analysis. X-ray diffraction analysis revealed that the title complex presents a 3D network constructed from Cu II –Schiff-base cations, 1D POM-MOF chains and solvent water molecules. Its water vapour adsorption isotherm at room temperature and pressure shows that the water vapour adsorbed by the complex is 51.67 cm 3 g –1 at the maximum allowable humidity, which corresponds to 7.1 water molecules per unit formula. In addition, it exhibits good proton conductivity (>10 –4 S cm –1 ) at 100 °C in the relative humidity range 35–98 %. The corresponding activation energy ( E a ) of conductivity was estimated to be 0.32 eV.
研究领域:
无机化学
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材料科学
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固体化学
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DOI
高影响因子
FUEL
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2016
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IF 3.611
Si-Wen Li,Rui-Min Gao,Rong-Lan Zhang,Jian-she Zhao
A catalyst system designed by a kind of hybrid material POM@MOF-199@MCM-41 (PMM) was found by a one pot and POM template self-construction of MOF-199 in the pore of MCM-41. This catalyst was exploited to act as a stable heteropolyacid-based one in the direct oxidative desulfurization process with a feedstock of model oil under O 2 as oxidant. Based on optimal conditions, the DBT conversion reached up to 98.5% and the PMM could be recycled ten times with a slight decrease, which was compared with heteropolyacid only based on MOF-199 and MCM-41, respectively. Additionally, the structure of ordered nano-sized pores of MOF-199 with POM encapsulated in was clear under crystal analysis, which offered strong evidences for the further movement into the MCM-41.
研究领域:
化学
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催化材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Xinlu Yang,Xinyu Xie,Siqi Li,Wenxuan Zhang,Xiaodan Zhang,Hongxiang Chai,Yuming Huang
Herein, we reported the design and fabrication of polyoxometalates coupling metal-organic framework (POM@MOF) hybrids derived hierarchical hollow Mo/Co bimetal oxides nanocages (Mo/Co HHBONs) for the peroxymonosulfate (PMS) activation to degrade levofloxacin (Lev). The Mo/Co HHBONs are hollow nanocages with high specific-surface areas and hierarchical micropores, mesopores , and macropores . In addition to compositional modulation, polyoxometalate (H 3 PMo 12 O 40 ·nH 2 O) exhibited striking effect on the textural properties of Mo/Co HHBONs. The Mo/Co HHBONs had outstanding catalytic activity with first order-kinetics that were 6 − 10 times higher those previously reported. They exhibited good adaptability over a pH range of 3 − 11, as well as excellent universality and reusability. By altering the surface porosity, electronic structure, and oxygen vacancies of Co 3 O 4 , hetero-metal Mo doping induced Mo/Co HHBONs significantly promote the generation of reactive oxygen species , including • OH, SO 4 •− , O 2 •− , and 1 O 2 . Density functional theory indicated that Mo/Co HHBONs had better adsorption, enhanced electron-transfer abilities, and a longer O-O bond length than did Co 3 O 4 , for improved catalytic reactivity. This research provides a new strategy to design the POM@MOF hybrids derived hierarchical hollow nanocages with highly PMS activating capacity for the removal of antibiotics and other refractory contaminants.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2025
·
IF 5.4
Biao Li,Yuqi Liu,Baizhuang Li,Yusi He,Yufeng Zhang,Xinying Wang,Yuebin Feng,Wei Li
Tetracycline (TC) antibiotics in aquatic environments pose severe ecological and health risks due to their difficult biodegradability and environmental accumulation. Persulfate-based advanced oxidation process (PS-AOP) has been proven to be a promising method for TC degradation in wastewater treatment but requires efficient, stable catalysts. Herein, three melamine-modified POM@MOF composites WCo@C-1, WCo@C-5 and WCo@C-10 (WCo-PMOFs and melamine in mass ratios of 1:1, 1:5, and1:10, respectively) were synthesized by calcining a mixture of WCo-PMOFs and melamine, which were used as catalysts for peroxymonosulfate (PMS) activation to degrade TC efficiently. The results demonstrated that the TC degradation rate by WCo @ C-10 activated persulfate (PMS) reached 95.83 % within 2 h superior to that of WCo@C-1 and WCo@C-5 under the same experimental conditions. Notably, the WCo@C-10/PMS system exhibited exceptional cycling stability, maintaining a degradation efficiency of 83.51 % even after four consecutive cycles. The X-ray photoelectron spectroscopy (XPS) and electrochemical impedance spectroscopy (EIS) characterization results indicate that the WCo@C-10 composite material exhibits outstanding catalytic performance. This characteristic is mainly attributed to the significant improvement in the material's dispersion and its having the smallest impedance arc radius among a series of materials, which reflects a lower charge transfer resistance and excellent electrical conductivity. These characteristics synergistically promote the efficient conversion of Co(III) to Co(II). The quenching experiment combined with electron paramagnetic resonance (EPR) analysis confirmed that superoxide radicals (O 2 ·- ) and singlet oxygen ( 1 O₂) are the main reactive oxygen species in this system. This study provides a new idea for designing efficient PMS-based advanced oxidation systems.
研究领域:
环境化学
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材料科学
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催化化学
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水处理技术
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环境污染与控制
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纳米功能材料
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自由基反应机制
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xiaojia Li,Yiyang Bai,Jingfang Li,Wenjia Qu,Liye Liang,Guangming Li
In this study, PW 5 V 7 @ rht -MOF-1 ( 1 ) was prepared via one-pot hydrothermal synthesis and its crystal structure was confirmed by X-ray diffraction analysis. To enhance catalytic performance, a series of defect-engineered PW 5 V 7 @ rht -MOF-1 ( 1-D x ) catalysts were further developed by using formic acid (FA) as a modulator. TG, PXRD, and BET analyses demonstrated that defects resulting from ligand deficiency in 1-D x enhanced their specific surface area and porosity, while maintaining the overall structural integrity. XPS, EPR and Py-IR analyses revealed the presence of additional oxygen vacancies and Lewis acid sites in 1-D 0.2 . Experimental results show that, with the assistance of the surfactant, the optimized catalyst ( 1-D 0.2 ) achieves 99.8% sulfur removal within 3 h at 100 °C, significantly improving upon the defect-free catalyst (71.1%). Cycle tests indicate that 1-D 0.2 maintains 93.4% desulfurization efficiency after seven consecutive uses, demonstrating its structural stability. In addition, the radical oxidation mechanism of the AODS reaction was further validated by radical scavenging experiments and EPR. This study presents a novel strategy for designing defect-engineered POM@MOF catalysts and demonstrates their application in deep fuel desulfurization, highlighting the crucial role of defect engineering in heterogeneous catalysis.
研究领域:
催化化学
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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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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2024
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IF 3.7
Na Chen,Yuan Li,Yang Pan,Haozhe Wang,Hao Gu,Yuan Sun,Tiedong Sun
The emergence of bacterial resistance has a negative impact on the conventional antimicrobial treatments, and research into the development of the new antimicrobial materials is of great significance. Multimodal synergistic antimicrobial materials exert better antimicrobial effects compared with a single modality. In recent years, Polyoxometalate (POM) has shown great potential in the biomedical field due to its high catalytic activity and high photothermal conversion ability. However, owing to its small surface area, its applications have been greatly limited. Herein, we designed a H 2 O 2 self-supplied CDT and PTT bimodal nanogeneration material (i.e., CaO 2 /POM@MOF) possessing a larger surface area for the treatment of the bacterial infections, in which CaO 2 could release O 2 and H 2 O 2 in the weakly acidic microenvironment of bacterial infection and the dual catalytic site of POM@MOF could enhance the CDT reaction to generate ROS, resulting in the bacterial oxidative stress and the leakage of the bacterial contents, and the exposure to the NIR light generates localized high temperature that cause the rupture of bacterial cell membranes and the denaturation of their proteins. Meanwhile, the superior stability of POM@MOF can release fewer metal ions to improve its biocompatibility. The in vitro antimicrobial experiments demonstrated that CaO 2 /POM@MOF possessed the combined CDT and PTT effect and exhibited excellent antimicrobial efficacy. This work presents a promising strategy to combat the bacterial infections.
研究领域:
生物医学
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材料科学
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微生物学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Xingyu Luo,Fengjiao Li,Fei Peng,Lizhen Huang,Xiaoling Lang,Meiqin Shi
Polyoxometalate encapsulated by metal–organic framework (POM@MOF) hybrid is an ideal precursor for electrocatalysts because it provides a homogeneous catalyst system with a flexible synergistic effect. However, controlling its fine structures to activate the derived catalyst after pyrolysis remains a challenge. The uniformly distributed carbon-defect tungsten oxides on the 3D carbon matrix were synthesized by using phospho-tungstic acid confined in HKUST-1 (PA@HKUST-1) as the precursor. By choosing ethanol as the solvent, the framework of PA@HKUST-1 was retained integrally and each pore of HKUST-1 kept intact even with holding the PA molecule inside. The well-organized structure of PA@HKUST-1 facilitated to offer a highly distributed metal source, and further transform into defect-rich catalyst. The average size of the resulting WOxCy/C catalysts was 1.5 nm, which was similar to a single molecule of PA. The WOxCy/C catalysts exhibited superior activity in the methanol oxidation reaction after being platinized due to the enhanced resistance to CO poisoning, which is also confirmed by DFT. This finding suggests a new route to design and achieve the defect-rich catalyst with controllable size.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2026
·
IF 19.9
Xiaoting Ren,Bing Yan,Lewang Yuan,Dalong Zhang,Zong-Jie Guan,Yu Fang
Optimizing carrier dynamics to elevate photocatalytic efficiency represents a central goal in the design of photocatalysts; however, achieving this remains a daunting challenge within the research community. In this study, we have devised and synthesized four types of intramolecular heterojunctions (POM@MOFs), constructed by integrating polyoxometalates (POMs) with metal–organic frameworks (MOFs). Specifically, we utilized an organic linker featuring a photosensitive phenothiazine core with incrementally oxidized sulfur sites, and employed Zn/Cd as the metal nodes to create four analogous POM@MOF composites, designated as SO x -M ( x = 1, 2; M = Zn, Cd). Through strategic heterointerface engineering, we have achieved a synergistic improvement in both the generation and separation efficiency of charge carriers within these materials. Our results demonstrate that the SO 2 -M series, which incorporates phenothiazine in a more oxidized state (-SO 2 -), surpasses the SO-M series (-SO-) in terms of charge carrier generation and separation efficiency. Furthermore, within the SO 2 -Cd , the covalent bonds connecting the MOF and POM components significantly facilitate the separation and migration of photogenerated electrons. This collaborative regulatory mechanism enables SO 2 -Cd to exhibit outstanding photocatalytic performance. This research introduces a pioneering approach for the cooperative modulation of oxidation states and heterointerface interactions, offering a promising pathway for the development of highly efficient photocatalysts.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Chenglong Wu,Jiulin Hu,Jing Tian,Fulu Chu,Zhenguo Yao,Yongjian Zheng,Dongguang Yin,Chilin Li
Mg anode has pronounced advantages in terms of high volumetric capacity, resource abundance, and dendrite-free electrochemical plating, which make rechargeable Mg-based batteries stand out as a representative next-generation energy storage system utilized in the field of large-scale stationary electric grid. However, sluggish Mg2+ diffusion in cathode lattices and facile passivation on the Mg anode hinder the commercialization of Mg batteries. Exploring a highly electroactive cathode prototype with hierarchical nanostructure and compatible electrolyte system with the capability of activating both an anode and a cathode is still a challenge. Here, we propose a POM⊂MOF (NENU-5) core–shell architecture as a hybrid precursor template to achieve the stacking of tailored chalcogenide nanosheets around MoO2-C conductive stakes, which can be employed as conversion–insertion cathodes (Cu1.96S-MoS2-MoO2 and Cu2Se-MoO2) for Mg–Li dual-salt batteries. Li-salt modulation further activates the capacity and rate performance at the cathode side by preferential Li-driven displacement reaction in Cu+ extrusible lattices. The heterogeneous conductive network and conformal dual-doped carbon coating enable a reversible capacity as high as 200 mAh/g with a coulombic efficiency close to 100%. The composite cathode can endure a long-term cycling up to 400 cycles and a high current density up to 2 A/g. The diversity of MOF-based materials infused by functional molecules or clusters would enrich the nanoengineering of electrodes to meet the performance demand for future multivalent batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）