CATALYSIS TODAY
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2024
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IF 5.2
Guiming Xie,Xingyang Bai,Fei Yu,Qingyuan Yang,Zhou-jun Wang
Three AuCu/ZnO bimetallic catalysts , AuCu/ZnO-BTC, AuCu/ZnO-BDC and AuCu/ZnO-MOF-74, were derived from various MOF precursors using facile hydrothermal methods . Among the resultant catalysts, the AuCu/ZnO-BTC catalyst possessed the best methanol synthesis activity, whose space time yield of methanol ( STY MeOH ) reached 359.0 g MeOH kg cat −1 h −1 at 250 °C under 3 MPa. Structural characterization reveals that in comparison with the AuCu/ZnO-BDC and AuCu/ZnO-MOF-74 catalysts, the AuCu/ZnO-BTC catalyst possessed higher specific surface area ( S BET ), tinier metal particle size, more oxygen vacancies , stronger metal-support interactions and larger amount of medium basic sites. In situ DRIFTS result demonstrates that formate (*HCOO) species were readily generated and bridged-methoxy (*b-OCH 3 ) species were selectively formed on the AuCu/ZnO-BTC catalyst, which may be related with its abundant oxygen vacancies and responsible for its superior methanol synthesis activity. The present work derives high-performance AuCu/ZnO bimetallic catalysts from MOF precursors and provides new insight into structure-activity relationships for CO 2 hydrogenation to methanol.
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DYES AND PIGMENTS
·
2024
·
IF 4.1
Ludan Shang,Shan Wu,Xinyu Liu,Yuhan Duan,Yanhui Li,Qian Duan
Molybdenum disulfide (MoS 2 ) is a nonlinear optical material with graphene-like structure. In order to further improve the nonlinear optical performance of MoS 2 and expand the application fields of MoS 2 , we report a simple in-situ self-growth method to functionalize MoS 2 nanosheets with metal-organic framework (MOF) for the first time to pursuit excellent reverse saturable absorption performance and optical limiting performance. Firstly, defective MoS 2 nanosheets was obtained by chemical etching with H 2 O 2 and cysteamine was inserted into the sulfur vacancies under ultrasound to obtain MoS 2 –NH 2 . Then 5,10,15,20-Tetra (4-carbomethoxyphenyl) porphyrin (TCPP) as MOF active growth sites were grafted on MoS 2 –NH 2 by amido linkage to obtain MoS 2 -TCPP in mild conditions. Finally, flower-like porphyrin-based CuMOF was grown on MoS 2 -TCPP by solvothermal method to obtain MoS 2 -CuMOF with stable structure. The third order nonlinear optical performance of MoS 2 -CuMOF were studied by Z-scan technique. It was found that the third order nonlinear absorption coefficient of MoS 2 -CuMOF was significantly improved compared with MoS 2 . Under the same energy of laser irradiation, the third order nonlinear absorption coefficient of MoS 2 -CuMOF nanocomposite in solution was 6 × 10 −10 m/W about 2.3 times of the pristine MoS 2 (2.6 × 10 −10 m/W). After blending the above materials with polymethyl methacrylate (PMMA) to prepare a solid device, the third order nonlinear absorption coefficient of MoS 2 -CuMOF/PMMA was 18 × 10 −10 m/W about 3.6 times of the MoS 2 /PMMA (5 × 10 −10 m/W). And MoS 2 -CuMOF/PMMA had better optical limiting ability than MoS 2 /PMMA. The significant improvement in the performance of the composites can be attributed to the energy transfer between MoS 2 and CuMOF, and porphyrin aggregation was inhibited by PMMA after the preparation of devices. Energy transfer can be proved by fluorescence spectroscopy. This work not only provided an example for the covalent functionalization of MoS 2 , but also offered a new method for designing materials with excellent nonlinear optical performance.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Lingyi Zhang,Jiachun Wu,Hongyun Xu,Huixia Li,Xiang Liu,Yanhua Song,Yanjuan Cui
The fabrication of non-metallic semiconductor heterojunction with superior redox capability for hydrogen (H 2 ) evolution from water and environmental remediation has been emerging as a prospective strategy. Herein, a novel two-dimensional (2D) g-C 3 N 4 /Ni-MOF Z-scheme heterojunction was prepared by a facile sonication-gel self-assembly method with g-C 3 N 4 and nickel metal-organic framework (Ni-MOF) nanosheets . The ultra-thin nanosheet structure of Ni-MOF was conducive to the formation of stable 2D heterojunctions. The opposite surface charge and matched band difference caused the charge flow from g-C 3 N 4 to Ni-MOF, resulting in an interfacial built-in electric field. The optimized NMF/CN-9 attained the optimal 3aphotocatalytic activity towards the degradation of tetracycline (TC) and H 2 evolution from water. Under visible light irradiation , the reaction rate for TC degradation (0.00497 min −1 ) and H 2 evolution (15.6 μmol·h −1 ) over NMF/CN-9 was nearly 2.4 and 2.1 folds higher than that of g-C 3 N 4 , respectively. Besides, the photocatalytic performance of NMF/CN-9 was also nearly 2 times higher than that of g-C 3 N 4 under simulated solar illumination. Such improvements were originated from higher photo-excited charge separation and superior redox ability derived from Z-scheme interfacial charge transfer. A possible photocatalytic mechanism was also proposed and the results indicated that efficient photo-induced electrons and reactive hole (h + ), superoxide radical (·O 2 - ) and hydroxyl radical (·OH) played a major role during the photocatalytic route. This work offers an intense insight into the construction of non-metallic semiconductor 2D heterojunctions for H 2 evolution and environmental wastewater treatment .
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Science Advances
·
2024
·Vol. 10
·期 16
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IF 11.7
Zherui Zhang,Yuhao Luo,Yuanhong Ma,Yaofeng Zhou,Dingcheng Zhu,Wanhua Shen,Junqiu Liu
The in situ generation of H2O2 in cells in response to external stimulation has exceptional advantages in modulating intracellular Ca2+ dynamics, including high controllability and biological safety, but has been rarely explored. Here, we develop photocatalyst-based metal-organic frameworks (DCSA-MOFs) to modulate Ca2+ responses in cells, multicellular spheroids, and organs. By virtue of the efficient photocatalytic oxygen reduction to H2O2 without sacrificial agents, photoexcited DCSA-MOFs can rapidly trigger Ca2+ outflow from the endoplasmic reticulum with single-cell precision in a repeatable and controllable manner, enabling the propagation of intercellular Ca2+ waves (ICW) over long distances in two-dimensional and three-dimensional cell cultures. After photoexcitation, ICWs induced by DCSA-MOFs can activate neural activities in the optical tectum of tadpoles and thighs of spinal frogs, eliciting the corresponding motor behaviors. Our study offers a versatile optical nongenetic modulation technique that enables remote, repeatable, and controlled manipulation of cellular and animal behaviors.
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npj Flexible Electronics
·
2025
·Vol. 9
·期 1
·1-11
·
IF 15.5
Liu Kai,Xu Yifan,Tian Xiaozhu,Liang Junxuan,Zhao Zhihui,Wang Jun,Zhang Ziqi,Zhang Kewei,Yang Song
Aiming at the poor selectivity of electrically conductive metal-organic framework (EC-MOF) chemoresistive materials, this study develops a breakthrough room temperature ammonia (NH 3 ) sensor by stacking ionically conductive MOF (IC-MOF) on an environmentally friendly biofabric. The synergism between ionic conductivity, tailored metal-nitrogen interaction, and fabric porosity enables the sensor with high response ( R 0 / R g = 14.7 towards 1 ppm NH 3 ), low detection limit (36 ppb), and remarkable selectivity (coefficient >5.12 against common organic interferents). Notably, the optimized sensor yields a sixfold enhancement in response as compared with traditional EC-MOF powders. A linear regression model validated by fivefold cross-validation achieves 98.4% accuracy in NH 3 concentration prediction, while the kNN classifier shows 96% accuracy in gas identification (tested on 192 samples). Preliminary clinical tests show that the sensor can clearly differentiate the exhaled NH 3 signals of four patients with HE from those of healthy individuals, demonstrating the potential for non-invasive diagnostics.
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Molecular Catalysis
·
2024
·
IF 3.9
Xiangsheng Zheng,Xiaohong Hao,Yan Wang,Siyu Gao,Dantong Wen,Jinchuan Wang
The development of novel biocatalysts is essential to promote the commercialization of biodiesel production by transesterification reaction. In this paper, Rhizopus oryzae lipase (ROL) was immobilized on an amino-functionalized zirconium-based metal organoskeleton by interfacial adsorption. The immobilization conditions were optimized and the enzymatic properties were tested, and the resulting novel biocatalysts exhibited higher stability and heat resistance. SEM, XRD and BET analyses were used to characterize the biocatalysts and carrier materials. The catalytic performance of ROL@UiO-66-NH 2 in the production of biodiesel by transesterification reaction was explored, and the production process was optimized by response surface method. The results showed that the conversion rate of FAEE reached 82.05% at molar ratio of ethanol/oil of 15.43:1, reaction temperature of 50.28°C, reaction time of 120.9 min, DES addition of 48.08 wt%, biocatalyst addition of 3 wt%, and ultrasonic power of 90 W. In addition, ROL@UiO-66-NH 2 demonstrated good recyclability, with the catalytic efficiency remaining at 71.87% after five cycles.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Na Zhang,Hang Zhao,Chuying Zhang,Haotong Guo,Zhi-Min Dang,Jinbo Bai
Polymer dielectrics are crucial for electrostatic energy storage and offer broad application prospects in advanced high-power electrical systems, but their energy storage performance declines considerably due to increased conductivity at elevated temperatures. This work presents a structurally-simple high-temperature composite dielectric by incorporating positively charged ultrafine UIO-66 nanoparticles into polyetherimide (PEI) matrix. Be distinguished from traditional sub-micron MOF structures that usually reported in very recently, the newly-found nanoscale effect endows the ultrafine UIO-66 (∼12.9 nm) with largely-increased active sites, surface charge density and electron affinity. These ultrafine UIO-66 nanoparticles can capture free charge through strong electrostatic interactions and introduce deeper traps in composite dielectrics, reducing conduction loss and improving energy storage property significantly at elevated temperatures. Specifically, filling only as tiny as 0.5 wt% ultrafine UIO-66 endows the PEI-based composite with ultra-high energy densities of 5.9J cm −3 and 3.7 J cm −3 accompanied by high charge–discharge efficiencies of 91.4 % and 84.1 % at 150 ℃ and 200 ℃, respectively. These obtained performance in this work surpasses those of most previously reported mono-layered composite counterparts. This study provides a straightforward and effective strategy for designing high-temperature polymer dielectrics in advanced electrical and electronic systems, offering a new route for future applications and developments.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Siyu Guo,Yanzhi Cai,Laifei Cheng,Yibing Yuan,Yuhan Wang,Haiming Yu,Zhongyi Hu,Dengpeng Chen,Hudie Yuan
Metal–organic frameworks (MOFs) have attracted attention due to their designable structures. However, recently reported MOF microwave-absorbing materials (MAMs) are dominated by powders. It remains a challenge to design MOF/carbon nanotube (CNT) composite structures that combine the mechanical properties of self-supporting flexibility with excellent microwave absorption. This work involves the hydrothermal approach to grow Ni-MOF of different microstructures in situ on the CNT monofilament by adjusting the molar ratio of nickel ions to organic ligands. Subsequently, an ultraflexible self-supporting Ni-MOF/CNT buckypaper (BP) is obtained by directional gas pressure filtration technology. The BP porous skeleton and the Ni-MOF with a unique porous structure provide effective impedance matching. The CNTs contribute to the conduction loss, the cross-scale heterogeneous interface generated by Ni-MOF/CNT BP provides rich interfacial polarization loss, and the porous structure complicates the microwave propagation path. All factors work together to give Ni-MOF/CNT BP an excellent microwave absorption capacity. The minimum reflection losses of Ni-MOF/CNT BPs decorated with granular-, hollow porous prism-, and porous prism-shaped Ni-MOFs reach −50.8, −57.8, and −43.3 dB, respectively. The corresponding effective absorption bandwidths are 4.5, 6.3, and 4.8 GHz, respectively. Furthermore, BPs show remarkable flexibility as they can be wound hundreds of times around a glass rod with a diameter of 4 mm without structural damage. This work presents a new concept for creating ultraflexible self-supported MOF-based MAMs with hierarchical interpenetrating porous structures, with potential application advantages in the field of flexible electronics.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yuchen Zhao,Jingyun Guo,Bo Yang,Panyouwen Zhang,Xinyi Wan,Lei Wang,Pingwei Ye,Xinsheng Peng
Solar-driven interfacial water evaporation (SDIWE) technology is an promising way to solve the shortage of fresh water scarcity. However, it is still challenging to generate clean water from organic compound contaminated water through SDIWE. Herein, a 3D multilayer inverted cone solar evaporator based on flexible MOF/graphene oxide composite membrane (CFG membrane) is designed for efficient water evaporation and purification. The Co-Ferrocene (Co-Fc) MOF loaded in the CFG membrane expands the interlayer spacing of GO, providing channels for water transport and enhancing the photothermal performance. The 3D multilayer inverted cone structure enhances the absorption of sunlight through multiple reflections of light between different layers. Based on the above design, the 3D evaporator with three layer CFG membranes demonstrates an evaporation rate of 2.28 kg m-2 h-1 under 1-sun illumination, good salt-resistance and long-term stability. Meanwhile, the Co-Fc MOF in the evaporator acts as an effective Fenton catalyst and promote the generation of ˙OH for the degradation of organic pollutants in wastewater. The degradation rate of pollutants in mixed wastewater (MB: 80 mg L-1; TC: 40 mg L-1; phenol: 40 mg L-1) by CFG-3 evaporator is all over 95%. Almost no volatile organic compounds (VOCs) were detected in the distilled water. This may provide a promising strategy for the efficient solar-driven evaporation and treatment of organic wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yaping Yan,Xiuyun Liu,Xiaojuan Wang,Haiyan Wen,Gang Wang,Liang Dai,Suxia Gao,Tingting Zhang,Bigui Wei
Urban stormwater runoff is a primary source of microplastic pollution in aquatic environments, and its efficient removal is critical for maintaining water ecological security. In this study, a superhydrophobic silica sand composite with MOF structure (HDTMS@ZIF-8@PDA@QS) was developed to enhance microplastic removal through hydrophobic interaction. The adhesion of the substrate was enhanced by polydopamine (PDA) coating, the rough structure and adsorption sites were provided by in-situ growth of ZIF-8 nanoparticles, and the superhydrophobicity was improved by HDTMS modification. Stability tests demonstrated that the material retained superhydrophobicity (WCA > 150°) under extreme temperature (−20 °C), high salinity (3.5 wt% NaCl), and a broad pH range (1−13). After mechanical abrasion, the WCA decreased by only 5 %. Self-cleaning experiments confirmed superior anti-fouling performance against both solid and liquid contaminants. Adsorption experiments revealed that the removal efficiencies of HDTMS@ZIF-8@PDA@QS for polypropylene (PP), polyethylene (PE), and polyethylene terephthalate (PET) microplastics (25 μm) were 98 %, 96 %, and 86 %, respectively, following the order of PP > PE > PET. The maximum adsorption capacity reached 67 mg/g, and after five cycles, the removal efficiency remained above 90 %. AFM and XDLVO theoretical analysis indicated that hydrophobic interaction was the main mechanism of microplastic adsorption, and the adhesion force between modified quartz sand and microplastic was more than four times that of pristine quartz sand. The MOF-based functional filter material proposed offers an efficient and sustainable strategy for mitigating microplastic pollution in urban stormwater runoff. This material holds significant potential for application in green infrastructure systems such as constructed wetlands and bioretention facilities.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yi Yao,Zixin Gao,Zhongjie Pan,Yanping Zhong,Lili Qin,Kexin Zhao,Shuhan Liu,Shengqing Zhang,Haoyang Han,Feiying Yin,Ruizheng Liang,Jinmin Zhao,Li Zheng
Platinum (Pt)-based nanozymes that effectively exert antioxidant effects exhibit great potential in the treatment of osteoarthritis (OA). However, these nanozymes are easy to agglomerate and have low catalytic efficiency, which can hardly meet the criterion of clinical therapy. To achieve efficient ROS removal, this study develops a novel ultrasound (US)-responsive piezoelectric nanozyme (MOF(Hf)-Pt) based on Pt with multi-enzyme mimicking activities and metal-organic frameworks (MOFs) with excellent piezoelectric properties. Results show that MOF(Hf)-Pt has excellent piezocatalytic enzyme activity, which can be adjusted by varying the intensity and time of US. Mechanistically, MOF(Hf)-Pt can increase ATP output and restore mitochondrial function, thereby reducing inflammatory factor levels. In vivo studies also reveal that under suitable US action, MOF(Hf)-Pt nanozymes can effectively inhibit the deterioration of OA, with reductions in OARSCI scores of 76.90 % and 82.66 % after 4 and 8 weeks, respectively. Particularly, the piezoelectric catalytic effect generated by MOF(Hf)-Pt can reverse oxidative stress-induced articular cartilage damage and promote cartilage regeneration, making it a promising candidate for OA treatment.
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COMPOSITES COMMUNICATIONS
·
2025
·
IF 7.7
Yue Lian,Hong Chen,Yanwen Xiao,Qiaoyu Huang,Zhaoxia Chen,Sijing Jiang,Yuhong Zhang
The increasing contamination of water resources by oily wastewater and human activities necessitates the development of efficient strategies for the remediation of polluted water sources. Due to the diversity of pollution sources, such as industrial wastewater, organic dyes, bacteria, and other complex pollutants, it is meaningful to develop a material capable of simultaneously treating these pollutants. The hydrophobic melamine sponge (PDMS@F-MOF@MS) was prepared using a simple impregnation method using zirconium metal-organic framework (UiO-66-NH 2 ), 1H,1H,2H,2H-perfluorodecyl trichlorosilane (FDTS), and polydimethylsiloxane (PDMS). The obtained PDMS@F-MOF@MS demonstrates remarkable superhydrophobic with a water contact angle of up to 156°. In addition, the PDMS@F-MOF@MS has robust adsorption capacity for a variety of organic solvents/oils (capable of absorbing 14.44 to 41.83 times its weight), a separation efficiency rate surpassing 95.9 %, and the ability to effectively separate oil-in-water emulsions. Furthermore, PDMS@F-MOF@MS demonstrates good mechanical properties and chemical stability, as well as good antibacterial and photocatalytic degradation properties. This project offers a valuable guide for the creation of versatile oil-water separation materials that can separate oil and water in variety of oily wastewater.
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危险品化学品经营许可证（带存储）