Nano Research
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2024
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IF 9.5
Xie Mingkuan,Xiao Xin,Wu Duojie,Zhen Cheng,Wu Chunsheng,Wang Wenjuan,Nian Hao,Li Fayan,Gu Meng Danny,Xu Qiang
High-entropy alloy (HEA)-based materials are expected to be promising oxygen electrocatalysts due to their exceptional properties. The electronic structure regulation of HEAs plays a pivotal role in enhancing their elctrocatalytic ability. Herein, PtFeCoNiMn nanoparticles (NPs) with subtle lattice distortions are constructed on metal-organic framework-derived nitrogen-doped carbon by an ultra-rapid Joule heating process. Thanks to the modulated electronic structure and the inherent cocktail effect of HEAs, the as-synthesized PtFeCoNiMn/NC exhibits superior bifunctional electrocatalytic performance with a positive half-wave potential of 0.863 V vs. reversible hydrogen electrode (RHE) for oxygen reduction reaction and a low overpotential of 357 mV at 10 mA·cm −2 for oxygen evolution reaction. The assembled quasi-solid-state zinc-air battery using PtFeCoNiMn/NC as air electrode shows a high peak power density of 192.16 mW·cm −2 , low charge–discharge voltage gap, and excellent durability over 500 cycles at 5 mA·cm −2 . This work demonstrates an effective route for rational design of bifunctional nanostructured HEA electrocatalysts with favorable electronic structures, and opens up a fascinating directions for energy storage and conversion, and beyond.
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Materials
·
2024
·Vol. 17
·期 10
·2195
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IF 3.1
Yu Liu,Panpan Li,Zegao Wang,Liangjuan Gao
This study reported a multi–functional Co0.45Fe0.45Ni0.9–MOF/NF catalyst for oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and overall water splitting, which was synthesized via a novel shape–preserving two–step hydrothermal method. The resulting bowknot flake structure on NF enhanced the exposure of active sites, fostering a superior electrocatalytic surface, and the synergistic effect between Co, Fe, and Ni enhanced the catalytic activity of the active site. In an alkaline environment, the catalyst exhibited impressive overpotentials of 244 mV and 287 mV at current densities of 50 mA cm−2and 100 mA cm−2, respectively. Transitioning to a neutral environment, an overpotential of 505 mV at a current density of 10 mA cm−2was achieved with the same catalyst, showing a superior property compared to similar catalysts. Furthermore, it was demonstrated that Co0.45Fe0.45Ni0.9–MOF/NF shows versatility as a bifunctional catalyst, excelling in both OER and HER, as well as overall water splitting. The innovative shape–preserving synthesis method presented in this study offers a facile method to develop an efficient electrocatalyst for OER under both alkaline and neutral conditions, which makes it a promising catalyst for hydrogen production by water splitting.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Linlin Yu,Qian Jia,Cailang Lu,Ruoyu Chen
The development of a multifunctional sponge with photothermal effect for adsorbing high-viscosity oil, as well as magnetic drive and excellent flame-retardant property, is significant in the field of oil/water separation, but also extremely challenging. In this work, a multifunctional MOF-based polyurethane (PU) sponge was successfully prepared using a simple method. Fe 3 O 4 -loaded NH 2 -MIL-101(Fe) nanoparticles were immobilized on PU sponge via low surface energy polydimethylsiloxane (PDMS) to obtain superhydrophobic NH 2 -MIL-101(Fe)@Fe 3 O 4 @PDMS@PU sponge (WCA = 155.6°), which exhibited excellent oil absorption, oil/water selectivity and reusability. The introduction of NH 2 -MIL-101(Fe)@Fe 3 O 4 endowed the modified sponge with excellent photothermal properties, which was manifested in that with the help of solar energy, the sponge heated up rapidly and could achieve efficient adsorption of high viscosity oil. The magnetic property of the modified sponge made it effectively separate oil and water mixture along a certain path under the control of a magnetic field. In addition, the NH 2 -MIL-101(Fe)@Fe 3 O 4 @PDMS coating made the sponge exhibit excellent flame retardancy, which could effectively improve the safety of the modified PU sponge in practical applications. In summary, NH 2 -MIL-101(Fe)@Fe 3 O 4 @PDMS@PU sponge has potential application prospects in the oil/water separation field.
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Small
·
2025
·
IF 12.1
Pengwei Tan,Shuyang Shen,Ying Zheng,Yushu Tang,Yuanyuan Luo,Zheng Zhang,Dong Men,Guotao Duan
Electrochemical transistor (ECT) biosensors can achieve ultrahigh sensitivity, while keeping challenges for large biomolecules due to their sizes over the thickness of the electric double layer (EDL) causing a failure of sensing reaction. Here, wafer-level Ni/Fe-metal-organic framework (MOF) films and corresponding ECT biosensors are fabricated for the detection of coronavirus nucleocapsid protein, which realize an ultralow detection limit of 1 fg mL −1 and a wide detection range of 1 fg mL −1 to 100 pg mL −1 . A 3D Debye space, originating from the unique stacking structure of nanosheets and nanoparticles in Ni/Fe-MOF film, is proposed to explain such ultrahigh sensitivity, which ensures the immune-binding and sensing process of the nucleocapsid protein large molecules located in the effective EDL space. Moreover, an appropriate Ni/Fe molar ratio is optimized to enhance the transmission of carriers, thus improving the signal-to-noise ratio and the sensing response. The Ni/Fe-MOF-ECT biosensors will find applications in highly sensitive detection for large biomolecules, and the 3D Debye space may be a design model for constructing other biosensors.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Wenqian Zhang,Shengming Zhang,Minghao He,Weixian Hu,Wenhao Han,Kangkang Zha,Qian Feng,Guohui Liu,Yanli Zhao,Bobin Mi
Postmenopausal bone loss due to estrogen deficiency necessitates effective therapeutic strategies. Our study explores targeting macrophage Aurora A kinase to mitigate bone loss. Aurora A kinase phosphorylation is observed being increased in bone marrow-derived macrophages (BMDMs) from ovariectomy (OVX) mice, along with a reduction in programmed death-ligand 1 (PD-L1) expression. Detailed analysis reveals that PD-L1 plays an immunomodulatory role by lowering the ratio of T helper 17 cells and regulatory T cells. The metabolic shift toward glycolysis through transcriptome sequencing, induced by Aurora A kinase inhibition, is essential for PD-L1 expression in BMDMs. The interaction between Aurora A kinase and cytochrome C oxidase subunit 5B is found to enhance PD-L1 expression. To apply these findings therapeutically, a multifunctional system is developed using a Nickel-metal organic framework combined with bisphosphonate and MLN8237 (BP@Ni-MOF/MLN8237). This system targets bone tissues through bisphosphonate and effectively delivers MLN8237 to macrophages, promoting PD-L1 expression for a favorable immune environment. Moreover, this system exhibits an obvious angiogenic effect. The present study highlights the crucial roles of macrophage Aurora A kinase and PD-L1 in maintaining bone homeostasis as well as the angiogenesis effect by Ni-MOF engineered system, presenting a promising therapeutic approach to prevent postmenopausal bone loss.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 12
·1-13
·
IF 5.3
Wang Xue,Zhao Zixuan,An Long,Wang Tianxiang,Yang Xiaojing,Shan Jiajia
An unlabeled electrochemical sensing strategy based on electroactive copper-centered metal–organic framework (Cu-MOF) film coupled with multiwalled carbon nanotubes (MWCNTs) was proposed for the rapid assessment of nanoplastic concentration. The sensing interface was fabricated via the electro-deposition of Cu-MOF on the pre-modified MWCNTs using the cathodic reduction method. The exposed copper active sites in Cu-MOF showed excellent electrochemical activity, which was further enhanced due to rapid electron transfer induced by highly conductive MWCNTs. Through the adsorption functionality of Cu-MOF film towards polystyrene (PS) nanoplastics, the rapid recognition for nanoplastics in aqueous solution was achieved, thereby causing the inhibition of the current response. The results showed a robust dependence of the inhibition rate on the PS mass concentration. The proposed detection method was used for the quantitative determination of PS nanoplastics with the sizes of 100 nm, 500 nm, and 1 μm. The applicability of this electrochemical sensing platform was successfully validated in real-world water sample analysis. Graphical abstract
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Journal of Materials Chemistry C
·
2024
·
IF 5.7
Shizhen Song,Tengfei Zheng,Bo Li,Hangcheng Yang,Qin-Xiang Jia,Zhuting Hao,Wen Zhang,Ying Zhang
Solvent vapor-driven soft actuators have been seen as promising devices for human-environment interaction and gained considerable attention in recent years. Considering the limited types of response solvent and the lack of quantification, MOF/polymer intelligent soft actuators may be a potential candidate of the fabrication of the bio solvent-driven actuators. Thus, this paper present a multiple solvent-driven soft actuator based on MIL-88B/PVDF asymmetric film, and also the comparison to the analogs based on other MIL-88(Fe) series flexible MOFs (including MIL-88A, 88C and 88D) was made for the deformation-structure relationship and the solvent-driven mechanism investigation. The deformation behavior to various organic solvent (including methanol, toluene and chloroform) of the MIL-88(Fe)/PVDF composite films have been investigated, and the structure and composition of the MIL88(Fe) fillers and the composite films were also characterized by SEM, FT-IR, and XRD. Based on the above results, the MIL-88B/PVDF composite which shows the diversity of response objects and the fast deformation response to most of the organic solvents through the solvent swelling/adsorption of the MOF skeleton, was used to fabricate a monolayer soft film composed by MIL-88B, carbon black (CB) and PVDF, namely MIL-88B/CB/PVDF. The MIL-88B/CB/PVDF film not only realizes the excellent deformation-discolor dual-responsive to methanol atmosphere with the visible deformation which could being quickly achieved within 1s under 10 vol % methanol atmosphere and the maximum crimp angle being up to 558o within about 50 s, and also a wide color change range including six view angle-dependent high saturation color (red, orange, yellow, green, blue and purple), but also shows an approximate linear relationship to three of the organic solvents (methanol, toluene and chloroform) between the maximum curl angle and the solvent concentration. Furthermore, several smart devices have also been fabricated, including the methanol-driven bionic petals, worm robot, alertor and LIG sensor. Therefore, such soft composites of flexible MOF and polymer have great potential in bio-robot and this work may provide new design strategy for the MOFs/polymer smart materials.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Fan Liu,Wenbo Li,Yuan Liang,Xianhua Zhang,Dongxiao Ji,Hengtao Liang,Mengyu Yuan,Yanchao Zhao,Haozhe Tang,Xiang Li,Jianxin He,Weili Shao
Functional materials that can quickly absorb and degrade mustard gas are essential for chemical warfare emergency response kits. In this study, a fiber membrane with excellent adsorption and catalytic degradation activity was developed by solution blow spinning polystyrene (PS)/polyurethane (PU) and hydrothermal in situ growth of a zirconium-based MOF (MOF-808). The mechanical properties of the PS/PU fibers were improved by adding a trimethylolpropane tris (2-methyl-1-aziridine propionate) (TTMA) cross-linking agent. Moreover, the C═O bonds in TTMA provided abundant growth sites for MOF-808 in the hydrothermal process, thereby greatly increasing the loading capacity. The fiber surface was completely covered with the MOF-808 particles within 24 h. The PS/PU/TTMA/MOF-808 fiber membrane was used for the catalytic degradation of 2-chloroethyl ethyl sulfide (CEES). The degradation efficiency reached 97.7% after 72 h, indicating its great application potential in emergency wiping cloths for mustard gas adsorption and degradation.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Suling Zhang,Hengli Liu,Defeng Fu,Hongting Zhao,Dong Zhang,Ting Lü
Metal–organic frameworks (MOFs) are promising materials for sample pretreatment. The performance improvement of powdered MOFs is hindered by their aggregation and difficult recovery. To overcome these issues, a biodegradable lightweight spherical aerogel was used as a support for the in situ growth of copper-based MOFs (MOF-199). Furthermore, Fe 3 O 4 nanoparticles were incorporated into the aerogel to achieve magnetic properties. Thus, hybrid aerogel spheres containing MOF-199 supported on magnetic oxidized cellulose nanofiber/carboxymethyl chitosan (MOF-199@mag-CNF/CMC) were fabricated. The effects of Fe 3 O 4 loading amount and organic-ligand concentration on the properties (spherical geometry and mechanical strength) of the hybrid aerogel spheres were studied. Their potential application in the extraction of benzodiazepines (BZPs) from urine samples prior to liquid chromatography–mass spectrometry was evaluated. The highly dispersed MOF-199 crystals on the spherical aerogel effectively overcame the inherent structural shrinkage of the bare aerogel spheres; thus, the MOF-199@mag-CNF/CMC aerogel spheres were robust and could withstand repeated use for at least eight consecutive extraction cycles. Further, MOF-199@mag-CNF/CMC exhibited improved BZP extraction efficiency, which was 2.5–11.6 times higher than that of bare Cu 2+ @mag-CNF/CMC aerogel spheres, primarily due to additional π–π interaction and H-bonding as well as improved specific surface area. Parameters influencing the extraction and desorption processes were also comprehensively investigated. Under optimal conditions, this method provided a wide linear range of 0.1–10 µg/L ( R 2 > 0.995) and good precision (2.8–6.7% for intra-day; 1.9–7.8 % for inter-day). The limits of detection and quantification ranged from 0.02 to 0.11 µg/L and from 0.06 to 0.33 µg/L, respectively. The recoveries for the urine samples spiked with three concentrations of BZPs ranged from 73.9 % to 114.1 %. The proposed method is simple, sensitive and eco-friendly and can be used for the determination of BZPs from urine for clinical and forensic examinations.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Guoxu Wang,Xiaomeng Fan,Fanfan Liu,Shoujiang Li,Wei Ding,Xiaoyan Liu,Chengbiao Wei,Feng Lin,Li-Zhen Fan
Ultra-thin, scalable solid-state electrolytes with high mechanical strength are essential for achieving high-performance all-solid-state lithium metal batteries (ASSLMBs). Among various types of solid-state electrolytes, composite solid electrolytes (CSEs) have emerged as an appealing option due to their ability to overcome the limitations of single-component solid-state electrolytes. In this study, ZIF-67 metal-organic framework (MOF) nanoparticles were self-assembled in situ on polyimide (PI) film fibers (referred to as PI@ZIF-67) to create continuous Li + transport channels. The ultra-thin, robust PI fiber film combined with MOF particles imparts high mechanical strength and excellent flexibility to the CSE. Additionally, the abundant sub-nanopores and surface Lewis acidic sites in ZIF-67 nanoparticles facilitate the dissociation of lithium salts and enhance the rapid transport of Li + . Consequently, 95% of the discharge capacity retention of the all-solid-state Li/PI 60 @ZIF-67-PEO/LFP cell was maintained after 300 cycles at 0.2C and 60 °C. Furthermore, an ultra-long lifespan of 3500 h at 0.2 mA cm -2 and 0.2 mAh cm -2 was achieved for the symmetric Li/PI 60 @ZIF-67-PEO/Li cell. The superior electrochemical performances are attributed to the effective Li + transport network and the high mechanical properties established by the continuous ZIF-67 particles within the PI 60 @ZIF-67-PEO CSE. This work presents a promising method for the integrated design of ultrathin CSEs that exhibit high ionic conductivity and exceptional mechanical robustness, making them suitable for ASSLMBs.
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CARBOHYDRATE POLYMERS
·
2024
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IF 10.7
Wenqian Nong,Honglin Luo,Gang Wang,Qicong Chen,Xiaosu Zou,Weiwei Miao,Jun Wu,Weiliang Guan,Shenhong Qu
The development of safe, environmentally friendly, edible antimicrobial packaging films represents a promising alternative to conventional plastic packaging for reducing spoilage and extending the shelf life of fresh food. Here, we propose a novel strategy to construct edible β-CD-MOF/carvacrol@zein (BCCZ) composite films by intertwining β-CD-MOF loaded with the antimicrobial essential oil carvacrol, and zein. The resulting BCCZ films exhibit high humidity-triggered, long-lasting bactericidal efficacy, effective fruit preservation, and excellent biosafety. Characterization revealed that BCCZ films possess a compact texture, hydrophilic surface, low water vapor permeability, and high humidity sensitivity. Additionally, this film act as a “storehouse” for carvacrol, enabling humidity-controlled release (96.3% release at 100% RH and only 12.0% at 43% RH on day 7). BCCZ film effectively inhibited Gram-positive Staphylococcus aureus , Gram-negative Escherichia coli , and fungi ( Botrytis cinerea ) through the release of liquid-phase and vapor-phase carvacrols under both direct contact and indirect contact conditions in high humidity. Owing to the film's humidity-triggered, long-term release of carvacrol, strawberries packed in BCCZ films maintained their freshness and appearance significantly better after seven days of storage at 21 °C. This work provides valuable insights and holds promise for the design and commercial application of safe, environmentally friendly freshness-preserving packaging films.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xu-Chao Xia,Feng Cheng,Peng Sun,Amare Aregahegn Dubale,Hao Han,En-Tian Cui,Jun Song,Xiu-Li Yang,Ming-Hua Xie
Photocatalytic CO 2 reduction is a potential promising strategy for eliminating the global energy crisis and environmental issue. However, the complex reduction pathway leads to multiple possible products with limited efficiency, representing a great barrier for the further development. Herein, we report a Metal-organic framework (MOF) based heterostructure model for the efficient photoreduction of CO 2 with full controllable product selectivity between CO and C 2 H 5 OH. Novel core-sheath like MOF@TiO 2 heterostructures could be efficiently prepared by the layer-by-layer (LBL) growth of HKUST-1 onto Cu-embedded TiO 2 nanofibers (NFs), affording covalent heterointerfaces for efficient S-scheme charge separation and promising potential in photocatalytic activity regulation. By improving the CO 2 capture and retention via in situ amino-functionalization of HKUST-1, the photocatalytic CO production rate could be greatly promoted from 8.76 ± 0.84 to 43.46 ± 0.86 μmol g −1 h −1 accompanied by an enhancement of selectivity from 91.7 % to 98.3 %. Moreover, the product could be efficiently engineered into ethanol with a C 2 product selectivity of 94.2 % by introducing Cu nanoparticles (NPs) as the additional C C coupling site. The in situ FT-IR and DFT calculations reveal the mechanistic process and decisive role of amino-functionalization and Cu NPs deposition in photocatalytic activity engineering. This work highlights the key factors and significance of fabricating MOFs based heterostructures with tunable photocatalytic activity for achieving CO 2 neutralization.
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危险品化学品经营许可证（带存储）