Journal of Materials Chemistry A
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2024
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IF 10.7
Ling-Xia Yun,Meng Qiao,Bin Zhang,Hang-Tian Zhang,Jie-Xin Wang
Utilizing plastic wastes as linker sources for metal–organic framework (MOF) synthesis is a green and sustainable methodology for the chemical upcycling of plastics. However, improving the depolymerization efficiency of polymers and avoiding highly corrosive solvents during the purification of the products remain significant challenges. Herein, we propose an approach to efficiently hydrolyze practical poly(ethylene terephthalate) (PET) wastes using aqueous dispersions of ultrasmall ZnO (6 nm) nanoparticles as the catalysts and subsequently synthesize five typical nano-MOFs by one-pot and two-pot strategies. The neutral hydrolysis of PET is greatly accelerated, with PET being completely depolymerized at 200 °C in 60 min with a terephthalic acid yield of 95.6%. The PET-derived MOF nanoparticles present high BET surface areas that are higher than or close to those of congeneric MOFs synthesized from petroleum-based and highly purified ligands. As a water absorbent, the two-pot MIL-101(Cr) exhibits high thermal stability with a water uptake capacity of 1327.3 mg g−1. For photocatalytic degradation of antibiotic pollutants, MIL-53(Al, Fe) samples derived from PET textiles show a high tetracycline removal efficiency of over 90% within 60 min without additives in an aqueous system, outperforming most of the conventionally prepared MOF catalysts. This approach disposes of discarded plastics in an eco-friendly way and produces value-added materials with excellent catalysis and adsorption properties.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
NANO
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2020
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IF 1.566
Aowen Li,Meimei Zhou,Pingping Luo,Jiaxin Shang,Pengbo Wang,Luxue Lyu
Nanofiber mats produced by electrospinning, with the advantages of specific surface area, porosity and chemical tenability, are an ideal support material for deposition of metal − organic framework (MOF) crystals. In this study, four types of MOFs (MIL-53(Al), ZIF-8, UiO-66-NH 2 and NH 2 -MIL-125(Ti)) were deposited on polydopamine (PDA)-modified electrospun polyvinyl alcohol (PVA)/SiO 2 organic − inorganic hybrid nanofiber mats by bulky synthesis. Because of the formation of Si–O–C–O–Si bridges between PVA chains and silica network, electrospun PVA/SiO 2 organic − inorganic hybrid nanofiber mats are quite stable in water or organic solvents and at high temperature are suitable as supports for MOFs deposition. The PDA layer, which exhibits a powerful adhesive ability to attach foreign objects, can effectively improve growth of MOFs on the surface of PVA/SiO 2 nanofiber mats. The obtained MOF composites combining the unique properties of electrospun nanofibers mats and MOFs particles become flexible and tailorable, greatly expanding the application range of MOFs materials. The synthesized MOF composites were used to adsorb chloramphenicol (CAP) in water. It was found that the four MOF composites could remove CAP from water effectively and MIL-53(Al) composite had the highest adsorption capacity due to the higher specific surface area.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
ACS Catalysis
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2020
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IF 12.35
Junli Guo,Lingling Yang,Zhida Gao,Chenxi Zhao,Ye Mei,Yan-Yan Song
Maintaining the high activity of an enzyme is a fundamental requirement to widen the application of metal–organic frameworks (MOFs) in the biotechnology, biosensor, and biomedicine fields. However, it is still challenging to monitor and understand an MOF environment-related activity for an enzyme. Here, we developed a MOFs-in-nanochannels configuration for broadening the biocatalytic activity of an enzyme in MOFs on demand. ZIF-8 [Zn(mim)2, Hmim = 2-methylimidazolated] grown in TiO2 nanochannels is used as the platform, and cytochrome C (CytC) is used as a model enzyme encapsulated in ZIF-8. The enzymatic catalytic process converts 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) to a positively charged product (ABTS+). On the basis of current–voltage properties, the change of ion transport characteristics in nanochannels can be monitored with time. The ZIF-8 encapsulating CytC molecules not only exhibit a significantly enhanced enzymatic activity in a wide temperature region (37–80 °C) but also have remarkably long storage stability at room temperature. The results of quantum mechanical calculation indicate that the Fe–S bond of CytC is inclined to break in the environment of ZIF-8 owing to the confinement effect of the MOF structure, favorable for enzymatic catalysis. The MOFs-in-nanochannel configuration provides an innovative and label-free design for the onsite monitoring of catalytic activity of an enzyme in MOFs, which holds great potential in constructing biosensing platforms with remarkable performance and stability.
研究领域:
生物技术
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生物传感
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生物医学
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DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
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2017
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IF 7.78
Yujie Yu,Chao Yu,Yazhen Niu,Jun Chen,Yilin Zhao,Yuchan Zhang,Rufei Gao,Junlin He
We designed an amplified detection strategy for the sensitive determination of lead ions (Pb 2+ ) based on a target-triggered nuclear acid cleavage of Pb 2+ -specific DNAzyme as a selectivity interface combined with Pd-Pt alloys modified Fe-MOFs (Fe-MOFs/PdPt NPs) hybrids acting as the signal tag. Streptavidin modified reduced graphene oxide-tetraethylene pentamine-gold nanoparticles (rGO-TEPA-Au) served as a sensor platform for immobilizing more DNAzyme. In the presence of Pb 2+ , the substrate DNA strand can be specifically cleaved at the ribonucleotide site by DNAzyme to produce a new single-DNA on the interface. Then, the hairpin DNA with hybrid strand matched by its complement to the single-DNA was employed to modify the Fe-MOFs/PdPt NPs bioconjugates for signal amplification . Fe-MOFs/PdPt NPs catalyze hydrogen peroxide (H 2 O 2 ) to produce the electrochemical signal which was recorded by chronoamperometry . Benefiting from the Pb 2+ -dependent DNAzyme, the proposed method can selectively detect Pb 2+ in the presence of other metal ions . The newly designed biosensor exhibited a good linear relationship ranging from 0.005 to 1000 nmol L −1 with a low detection limit of 2 pM (S/N = 3) for Pb 2+ . This Pb 2+ -dependent DNAzyme based ultrasensitive biosensor showed high sensitivity and selectivity, providing potential application for Pb 2+ detection in naturally contaminated sewage and spiked drinking water samples.
研究领域:
生物化学
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环境科学
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分析化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Li Xia,Wenxi Zhou,Yifan Xu,Zhengqiang Xia,Xinzhi Wang,Qi Yang,Gang Xie,Sanping Chen,Shengli Gao
The introduction of rich-electron ligands is a promising strategy to improve the ligand-to-metal charge transfer (LMCT) ability of metal–organic frameworks (MOFs) for efficient photocatalytic CO 2 reduction reactions (CO 2 RR), while the resulting impaired Lewis acid sites go against stable bonding with CO 2 and hinder the electron transfering to CO 2 . It is thus the key to search a trade-off between increasing LMCT and frustrating Lewis acid. Herein, the ferrocene (Fc) modified UiO-66 series MOFs, NH 2 -UiO-66-Fc, have been prepared to optimize LMCT for boosting CO 2 RR through a simple solvent-assisted ligand incorporation (SALI) method. Theoretical calculation and systematic experiments, including photoelectrochemical measures, in situ electron paramagnetic resonance, fluorescence probe analysis and X-ray photoelectron spectroscopy indicate that with increasing Fc content, the LMCT energy of MOFs significantly decreases from 2.66 to 2.10 eV based on the established electron transfer double-channel mechanism, while the Lewis acidity of Zr sites reduces with the CO 2 adsorption energy ( E ad ) ranging from −1.061 to −0.632 eV. Through introducing an optimal Fc content, NH 2 -UiO-66-Fc (2.0) integrating satisfactory LMCT ability and Lewis acidity shows superior photocatalytic CO 2 RR performance (CO yield: 90.65 μmol·g −1 ·h −1 ), about 13 times higher than that of the unmodified MOF and superior to most reported pristine MOF photocatalysts. DFT calculation demonstrates that the excellent performance of NH 2 -UiO-66-Fc (2.0) is attributed to the lowest energy barrier of 1.50 eV for the rate-limiting step of *COOH formation. In this work, such a simple post-modification strategy for facilitating the whole electron transfer path of photocatalytic CO 2 RR will provide a new way to construct high-performance MOFs-based CO 2 RR photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
CARBON
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2023
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IF 10.9
Mushan Yuan,Haoruo Zhang,Yang Fei,Junyu Lu,Junliang He,Baowei Qiu,Zhong Zeng,Hui Liu,Wenbin Chen,Mei Liang,Yang Chen,Huawei Zou
Developing an efficient EM wave absorbing material that can broadband absorb EM waves in a wide thickness range is a significant challenge. Herein, we report a multi-scale heterogeneous Co/C composite foam with a three-dimensional (3D) lamellar network to address this challenge. The internal structure of melamine foam (MF) is engineered via carboxymethyl cellulose (CMC) in-situ lamella formation to guarantee excellent impedance matching. Meanwhile, the CMC lamellar network extends the EM wave transmission path. The MOF-derived particles grow uniformly in the lamellar network, covering channels of EM wave transmission, which significantly enriches the EM wave loss mechanism and enhances attenuation capability. Benefiting from the synergistic effect of the 3D lamellar network and multi-scale heterogeneous carbon source, an EM absorber strikes a balance between impedance matching and absorption efficiency. As a result, Co/C@MC delivers an effective absorption bandwidth (EAB) that is more than 8 GHz in the whole range of thicknesses from 3.5 to 8 mm, Ni/C@MC exhibits an EAB of 8.5 GHz at 3.3 mm and Fe/C@MC shows the optimal reflection loss of −76.9 dB at 2.5 mm. This work provides a lamellar network/regional enhancement unit strategy for preparing ultra-efficient broadband EM wave absorbing materials.
研究领域:
材料科学
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电磁学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xiang Li,Xiaoge Chen,Bo Wang,Gang Yu
The development of engineered nanomaterials has aroused great attention in controlling the existence of toxic micropollutants. However, their performance in complex environmental matrices is frequently neglected. Highly efficient enrichment coupled with synergistic degradation with low concentrations is challenging but significant in practical industrial applications. In this study, a large group of active pharmaceutical compounds (PACs) at environmentally relevant concentrations ∼ μg/L were rapidly extracted in core-shell MIL-100 (Fe), followed by effective degradation during the visible-light photo-Fenton process in situ. Unexpectedly, in natural secondary wastewater, adsorption capacities were inhibited (2–50 % decreased after 60 min), while the degradation kinetics of eight PACs were remarkably promoted (1.42–2.92 times higher). Under neutral pH, the accumulated pharmaceuticals within cages were effectively decomposed by •OH and 1 O 2 , mainly derived from visible-light-induced reduction of Fe (III)-cluster and the generation of ROS. The structural parameters (log K ow ) were closely correlated to the adsorption behavior (R 2 = 0.74), which remarkably facilitated the degradation. The powder was loaded onto the PTFE/ultrafiltration membrane in a flow-through reactor. The targeted PACs were rapidly degraded over the self-cleaning surface under visible light irradiation, implying a promising future for industrial application.
研究领域:
环境科学
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纳米材料科学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Xiaoling Ma,Wenlong Wang,Chenggong Sun,Hui Li,Jing Sun,Xin Liu
In light of the promising merits of large surface area, uniform pore size, and tunable functional groups, metal-organic frameworks (MOFs) have great potential to be utilized for adsorbing volatile organic compounds (VOCs). In this study, three Fe-based MOFs, MIL-100(Fe), MIL-101(Fe), and MIL-53(Fe), were synthesized systematically and used to adsorb a typical VOC, toluene. Static adsorption, dynamic breakthrough curves , and adsorption kinetics were conducted to assess the adsorption performance. Additionally, the surface functional groups, pore structure, and morphology were systematically characterized by means of XRD , SEM, XPS, FTIR and N 2 adsorption-desorption analyses to reveal the cause of the difference in adsorption of these Fe-based MOFs. The results revealed that the maximum equilibrium adsorption capacity of 663 mg/g was achieved by MIL-100(Fe) with the highest specific surface area and pore volume. The dynamic adsorption of toluene on MIL-100(Fe) was in accordance with the pseudo-first order kinetic model and the Langmuir isothermal model. The formed π-π stacking interaction between organic ligands and the benzene ring in the MIL-100(Fe) cluster is the primary adsorption mechanism based on XPS analysis. Moreover, MIL-100(Fe) was easily regenerated via microwave irradiation with a negligible adsorption capacity decrease after three cycles. This work highlights the feasibility of hierarchical porous Fe-based MOFs as toluene adsorbents and promotes the application of MOFs in the field of pollution control .
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Chemosensors
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2024
·Vol. 12
·期 3
·39
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IF 3.7
Yu Zhang,Chang Liu,Rongqiu Yan,Chenghong Lei
Bipyridyl Ruthenium-decorated Ni-MOFs on multi-walled carbon nanotubes (MWCNT-RuBpy@Ni-MOF) were synthesized. In an alkaline solution, the glucose was electrocatalytically oxidized at +0.5 V vs. Ag/AgCl at the composite interface of MWCNT-RuBpy@Ni-MOF on a glassy carbon electrode. The Ni3+/Ni2+redox couples in Ni-MOFs played a key role as the active center for the catalytic oxidation of glucose at the electrode, where both RuBpy and MWCNTs enhanced the current responses to glucose. The resulting enzymeless glucose sensor from MWCNT-RuBpy@Ni-MOF exhibited a wide range of linear responses, high sensitivity and selectivity for the determination of glucose.
研究领域:
材料科学
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电化学
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纳米技术
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yong Xiang,Chang-Yuan Cheng,Kang-Fei Lu,Wen-Cai Bai,Zhou-Xuan Zang,Li Xu,Guo-Ji Liu
Traditional metal–organic frameworks, characterized by their micropore-dominated structures, suffer from severe pore channel blockage during gold ion recovery due to the aggregation of gold nanoparticles, significantly reducing the utilization rate of adsorption sites. To address this issue, we developed hierarchically porous MOFs through ligand removal and metal exchange strategies, precisely installing adsorption sites within meso/macropores to effectively prevent pore obstruction by adsorbed-reduced gold particles. Subsequent Metal substitution further enhanced the material’s aqueous stability, enabling retention of 93 % adsorption capacity after 5 cycles while preserving the precisely engineered pore structure. The functionalized HP-MOF-5/DU achieves an ultrahigh Au(III) capacity of 1566 mg/g, rapid kinetics, and exceptional selectivity. Practical validation demonstrates 85 % gold recovery from real electronic waste leachates, with calcination yielding gold particles of 23.7 K purity. Through rational regulation of pore channel structures at adsorption sites, we have significantly enhanced the material’s Au(III) adsorption performance, pioneering a novel direction for the design of reducible metal-targeted adsorbents.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
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2022
·Vol. 12
·期 55
·35666-35675
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IF 4.036
Junhao Hu,Qiong Yi,Ziyi Xiao,Feng Tian,Tingting Shu,Xiaolan Liu,Yingxi Wang,Ling Li,Jiangang Zhou
Doxorubicin (DOX) has been an emerging environmental pollutant due to its significant genotoxicity to mankind. Advanced oxidation processes are a potential strategy to remove DOX in water solution. To develop a highly efficient catalytic agent to remove DOX, bimetal MOFs were synthesized, with Cu2+ and Co2+ as the central ions and adenine as the organic ligand. This study investigated the degradation of DOX by Co/Cu-MOFs combined with peroxymonosulfate (PMS). It was found that the degradation of DOX by Co/Cu-MOFs can reach 80% in only 10 seconds. This can be explained by the charge transfer from Co(III) to Co(II) being accelerated by Cu2+, resulting in the rapid generation of free radicals, which was proved by the EIS Nyquist diagram. Co/Cu-MOFs can be reused by simply washing with water without inactivation. Therefore, Co/Cu-MOFs can be used as an efficient catalytic agent to degrade DOX in environmental water.
研究领域:
环境科学
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材料科学
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药学
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产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
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2023
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IF 9.4
Shengnan Lin,Tingan Zhang
With the upgrading of mobile and portable electronic devices, people have higher requirements for the performance of batteries , and anode materials, as one of the factors affecting the electrochemical performance of lithium ion storage, have become a hot spot of widespread concern. This paper illustrates a creative and effective strategy to synthesize four different NiCo-MOFs materials. After studying their respective unique structural features, it was found that, unlike the topologies of NiCo-PTA (terephthalic acid) and NiCo-H 3 BTC (trimesic acid), the substitution of Ni and Co for N occurred in NiCo-EDTA (ethylenediaminetetraacetic acid) and NiCo-BI (benzimidazole). Electrochemical studies show that NiCo-PTA, NiCo-EDTA, NiCo-H 3 BTC, and NiCo-BI all have high initial discharge specific capacities of 1770.41576.11905.1 and 1877.5 mAh/g at a current density of 100 mA/g. When NiCo-EDTA and NiCo-BI are cycled at a current density of 100 mA/g, the specific capacity decreases more slowly than NiCo-PTA and NiCo-H 3 BTC. Similarly, the capacity of NiCo-PTA and NiCo-H 3 BTC almost began to rise at the 70th cycle, the capacity of NiCo-BI began to rise at the 67th cycle, and NiCo-EDTA showed the slowest rise at the 78th cycle, they all showed excellent cycle performance.
研究领域:
材料科学
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能源存储与转换
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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）