APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Weiwei Li,Wenlan Ji,Murat Yılmaz,Tian C. Zhang,Shaojun Yuan
Arsenic is a toxic carcinogen, and arsenic pollution in groundwater is one of the most serious environmental problems in the world. Thus, it is an urgent problem to efficient removal of arsenic from groundwater. In this work, a novel MWCNTs/MIL-53(Fe) nanocomposite was successfully synthesized to improve the water stability of MIL-53(Fe) by incorporation of carboxylated multi-walled carbon nanotubes (MWCNTs) using a one-pot hydrothermal method, and was then used to efficiently adsorb As(V) ions from groundwater. Adsorption experimental results demonstrated an ultrafast adsorption rate of As(V) on the MWCNTs/MIL-53(Fe) nanocomposites in solution pH values of 3 to 10, and the adsorption equilibrium could be reached in circa 20 min with an adsorption capacity of 27.24 mg·g −1 in a low As(V) concentration of 10 mg·L −1 . The adsorption kinetics of As(V) on the MWCNTs/MIL-53(Fe) was found in line with the pseudo-second-order (PSO) kinetic model, and was simultaneously controlled by both internal diffusion and liquid film diffusion. The adsorption isotherm data conformed to the Redlich-Peterson isotherm model, indicating both physical and chemical adsorption occurred at heterogeneous interfaces. Moreover, the postulated adsorption mechanism of As(V) on MWCNTs/MIL-53(Fe) nanocomposites was ascribed to hydrogen-bond interaction, electrostatic attraction and chemical complexation. Therefore, the as-prepared MWCNTs/MIL-53(Fe) nanocomposites not only exhibit superior water stability and outstanding adsorption performance in removing arsenic-contaminated groundwater, but also offer a novel insight for rational preparation of water-stable MOF-based composites.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yulong Bian,Bin Liu,Shuang Liang,Binbin Ding,Yajie Zhao,Fan Jiang,Ziyong Cheng,Abdulaziz A. Al Kheraif,Ping'an Ma,Jun Lin
Nowadays, the therapeutic efficiency of tumor can be significantly influenced by the limitation of endogenous tumor microenvironment (TME). An ideal solution for improving therapeutic efficiency is constructing TME-responsive and multifunctional nanoreactor. Herein, a TME-responsive nanoreactor has been constructed using novel dendritic mesoporous silica nanoparticles (DMSNs) as the cornerstone, followed by anchoring platinum-(IV) prodrugs, loading photosensitizer indocyanine green (ICG), and decorating Cu 2+ carboxylate MOFs. The prepared nanoreactor provides a high loading efficiency for Pt prodrugs and ICG, while the externally decorated MOFs can prevent premature leakage in neutral physiological environment at the same time. However, after accumulation at the tumor site, the outer MOFs can be rapidly decomposed in the TME to release Cu 2+ , which achieves efficient chemodynamic therapy (CDT) through Cu 2+ -triggered Fenton-like reaction and GSH depletion ability. At the same time, the released Pt drugs can achieve efficient chemotherapy. Moreover, the near-infrared (NIR) can activate the photodynamic and photothermal therapy (PDT&PTT) ability of ICG, resulting in PTT-enhanced CDT. Meanwhile, the nanoreactor can exhibit photothermal and magnetic resonance imaging (MRI) ability for highly specific diagnosis of tumor. Overall, this study provides a paradigm of TME-responsive nanoreactor for collaboratively multimodal enhanced tumor therapy.
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Journal of Environmental Sciences
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2022
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IF 6.796
Ping Chen,Yalan Wang,Xiaoqin Zhuang,Haijin Liu,Guoguang Liu,Wenying Lv
Zr-based metal-organic frameworks (MOFs) have been developed in recent years to treat heavy metals, e.g. hexavalent chromium Cr 6+ pollution, which damages the surrounding ecosystem and threaten human health. This kind of MOF is stable and convenient to prepare, but has the disadvantage of low adsorption capacity, limiting its wide application. To this end, a novel formic acid and amino modified MOFs were prepared, referred to as Form-UiO-66-NH 2 . Due to the modification of formic acid, its specific surface area, pore size, and crystal size were effectively expanded, and the adsorption capacity of Cr 6+ was significantly enhanced. Under optimal conditions, Form-UiO-66-NH 2 exhibited an excellent adsorption capacity (338.98 mg/g), ∼10 times higher than that reported for unmodified Zr-based MOFs and most other adsorbents. An in-depth study on the photoelectronic properties and pH confirmed that the adsorption mechanism of Form-UiO-66-NH 2 to Cr 6+ was electrostatic adsorption. After modification, the improvement of Cr 6+ adsorption capacity by Form-UiO-66-NH 2 was attributed to the expansion of its specific surface area and the increase in its surface charge. The present study revealed an important finding that Form-UiO-66-NH 2 elucidated selective adsorption to Cr 6+ in mixed wastewater containing toxic heavy metal ions and common nonmetallic water quality factors . This research provided a new acid and amino functionalization perspective for improving the adsorption capacity of Zr-based MOF adsorbents while simultaneously demonstrating their pertinence to target contaminant adsorption.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Fei Wu,Mengyun Ling,Lingyun Wan,Pei Liu,Yabin Wang,Qiuyu Zhang,Baoliang Zhang
Herein, we construct two metal–organic frameworks (MOFs) composite nanoflowers (NFs) with anisotropic binary assembled structures by a facile one-pot method. Different from the two-step epitaxial growth method, the anisotropic assembly of the binary MOFs (MOF-5 and MIL-88B) in the mixed system can be realized without preparing the template MOFs. The ions coordinated self-assembling behaviors during the formation of the three-dimensional (3D) structure are clarified. The absorbing mechanisms of the derivative absorber are elucidated. The results indicate that the special hierarchical assembled structure endows absorbers with rich heterogeneous interfaces, porous structure, suitable impedance matching and complementary loss mechanisms. The optimized absorbers FeCoZn@C NFs and FeNiZn@C NFs exhibit outstanding microwave absorption performance. Only with a matching thickness of 1.9 mm, the effective absorbing bandwidth (EAB, reflection loss (RL) < −10 dB) of the absorber covers 6.0 GHz (12–18 GHz, the entire Ku band). The minimum reflection loss (RL min ) reaches −53.1 dB (loss of electromagnetic waves above 99.999%). This study might shed light on the preparation of high-performance microwave absorbers with sophisticated structures.
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BIOELECTROCHEMISTRY
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2022
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IF 5.76
Axin Liang,Shanshan Tang,Miao Liu,Yue Yi,Bingteng Xie,Huipeng Hou,Aiqin Luo
Human IgG is one of the most important immunoglobulins in the human body. The present study described the fabrication of four kinds of layer-by-layer structures of copper metal-organic frameworks (Cu-MOFs) on the working electrode by electrodeposition, which were then applied as an electrochemical sensor for the sensitive determination of IgG in serum. First, MOFs synthesized using different deposition potentials are expected to have varied morphology and properties. Herein, four copper MOFs (Cu-MOFs) were electrosynthesized by a simple and direct reduction approach. The as-synthesized Cu-MOFs exhibit varied morphology and electrocatalytic behavior. Then, IgG was employed as a template in the electropolymerization of pyrrole-imprinted films on the surface of glassy carbon electrodes. Finally, the template protein was removed to form a molecularly imprinted film with the capability to qualitatively and quantitatively signaling of IgG. Under optimized conditions, the sensor for IgG exhibits a wide detection range of 0.01–10 ng mL −1 with a limit of detection (LOD) of 3 pg mL −1 (S/N = 3). Besides, other parameters including the selectivity, reproducibility (RSD 3.6%), and recovery rate (95.2–102.0%) are all satisfactory. The practicability of the sensor was verified by detecting IgG in human serum samples, which indicated that the sensor was suitable for potential clinical applications.
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高影响因子
FOOD CHEMISTRY
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2022
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IF 9.231
Fuxiang Wang,Zuopeng Li,Hongping Jia,Runhua Lu,Sanbing Zhang,Canping Pan,Zhiqiang Zhang
A turn-on fluorescent sensing platform based on an ultralow concentration of Al-metal organic frameworks for the detection of aflatoxin B 1 has been developed for the first time. This fluorescence turn-on sensor exhibits the largest fluorescence enhancement (or quenching) constant value of 179404 M −1 among all luminescence-based chemical sensors reported till date. Moreover, the sensor afforded a rapid detection of aflatoxin B 1 , with a linear response in the concentration range of 0.05–9.61 μM and a low detection limit of 11.67 ppb. Additionally, the fabricated sensor showed good repeatability, reproducibility, stability, and selectivity. Most importantly, the practical application of this sensor has been demonstrated by detecting aflatoxin B 1 in complex tea samples with low relative standard deviation (≤7.72%; n = 3) and satisfactory recoveries. In summary, the proposed method has great potential as a simple, sensitive and selective strategy for monitoring aflatoxin B 1 in food samples.
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高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Haoquan Wang,Shan Su,Tao Yu,Chunfeng Meng,Hu Zhou,Wenjia Zhao,Shitan Yan,Ting Bian,Aihua Yuan
Rational design of metal/metal oxide hybrids embedded in heteroatom-doped carbon is a desired strategy to improve the kinetics of oxygen reduction (ORR)/evolution (OER) reactions. Herein, we present an elaborate method for preparing FeNi-based bimetallic alloy/oxide hybrids implanted in spongy-like N-doped carbon (S-FeNi/NiFe 2 O 4 @NC) via introducing FeNi Hofmann-type metal-organic frameworks (MOFs) as pyrolysis precursors. Impressively, the evenly distributed FeNi alloys coexisting with oxides are directly derived from bimetallic nodes in the MOFs, which are expected to boost the intrinsic electrocatalytic activity by multi-compositional synergism. Meanwhile, spongy-like N-doped carbon matrix would be effective for achieving rich metal active sites and rapid mass/electron transport. Accordingly, the obtained S-FeNi/NiFe 2 O 4 @NC-800 shows an extraordinary electrochemical activity with an ORR/OER potential gap of 0.76 V. In addition, the catalyst emerges outstanding stability with potential losses that are only half those of commercial reference catalysts for both ORR and OER after 10,000 cycles. Importantly, zinc-air battery assembled with S-FeNi/NiFe 2 O 4 @NC-800 delivers a high peak power density of 129 mW cm −2 and an excellent specific capacity of 837 mA h g −1 .
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 13
·4247
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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
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TALANTA
·
2022
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IF 6.556
Wei Huang,Yao Chen,Lingyan Wu,Mei Long,Zhifeng Lin,Qianqian Su,Fuli Zheng,Siying Wu,Huangyuan Li,Guangxia Yu
L-tryptophan (Trp) is an essential amino acid for humans and plays crucial roles in many metabolic functions. Trp levels can be used for diagnosing different kinds of metabolic disorders and the symptoms associated with those diseases. Herein, a novel, simple and sensitive sensor based on 3D peony-like bimetallic conductive MOFs (Co–Ni-MOFs) was fabricated for the electrochemical determination of Trp. The bimetallic conductive MOFs were synthesized by a facile one-pot hydrothermal process. On account of the synergy between the Ni 2+ and Co 2+ ions, the bimetallic Co–Ni-MOFs showed excellent electrochemical performance, including good conductivity, large effective surface areas, and high electrocatalytic reactivity toward the oxidation of Trp. Consequently, the Co–Ni-MOFs-modified electrodes obtained a wide linear range from 10 nmol L −1 to 300 μmol L −1 and a low detection limit of 8.7 nmol L −1 (S/N = 3) for Trp. Additionally, the prepared sensor also displayed high selectivity, long-term stability and reproducibility. Moreover, the proposed sensor was successfully applied to determine the levels of Trp in the plasma of mice after cadmium intoxication.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Cheng Zeng,Yan Wang,Tong Xiao,Zhicheng Yan,Jinquan Wan,Quanmo Xie
To improve the efficacy of organic pollutant removal using sulfate radicals, we designed MIP@C-Fe-Nx, a molecularly imprinted material capable of targeting the degradation of tetrabromobisphenol A (TBBPA), which can be used as both adsorbent and catalyst to recognize and degrade Tetrabromobisphenol A (TBBPA) accurately, and the final removal rate of TBBPA can reach 104.6 mg·g −1 . Based on the synergistic effects of MIP@C-Fe-Nx on the excellent organic pollutant recognition and catalytic performance, low concentrations of TBBPA can be pre-targeted, concentrated, and fixed on the surface of MIP, and degraded simultaneously in-situ by·OH and SO 4 •- which are produced by activating PS with C-Fe-Nx. Recognition experiments demonstrated that MIPs had perfect performance in recognizing and adsorbing TBBPA and debromination intermediates. The DFT calculations and HPLC-MS analysis indicated that MIP@C-Fe-Nx had a targeted recognition and accumulation for TBBPA and debromination intermediates, for example, dibromobisphenol A, monobromobisphenol A, and bisphenol A, thus avoid the formation of toxic intermediates causing secondary contamination.
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高影响因子
CARBON
·
2021
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IF 9.594
Zhen Xiang,Xiang Zhang,Yuyang Shi,Lei Cai,Jie Cheng,Haojie Jiang,Xiaojie Zhu,Yanyan Dong,Wei Lu
Developing high-efficiency electromagnetic wave absorption materials with versatility has been a hotspot and it remains a huge challenge. Here, we reported versatile laminated Ni nanoparticles @ porous carbon (Ni@C) nanocomposites synthesized by a facile carbonization of Ni-based metal-organic frameworks (MOFs) precursor. It was found that the phase components (Ni and C phases) and nano/microstructure (laminated and porous characterizations) were well-modified by controlling the calcination temperature, which led to the variation of the degree of graphitization , magnetic properties , and electromagnetic performances. It showed that the laminated porous Ni@C nanocomposites achieved enhanced microwave absorption performances with a thin thickness of 1.5 mm, a strong reflection loss of −59.8 dB and an effective absorption bandwidth of 4.5 GHz. The underlying microwave absorption mechanism was owing to the improved synergistic effects of polarization relaxation, electron transport , ferromagnetic resonance, as well as multiple reflections and scattering in the laminated porous Ni@C nanocomposites. Furthermore, the multicomponent and laminated porous architecture endowed nanocomposites with favorable waterproof, heat isolation and infrared shielding versatility. Therefore, this work demonstrated a facile approach to develop MOFs-derived versatile laminated porous nanocomposites with efficient microwave absorbing performances.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Fang Li,Yuhui Tian,Shibiao Su,Changshui Wang,Dong-Sheng Li,Dandan Cai,Shanqing Zhang
High performance and cost-effective electrocatalysts are crucial to the oxygen evolution reaction (OER) in water splitting. Herein, we use density functional theory (DFT) calculation to systematically explore the catalytic activities of single-metallic organic frameworks (s-MOFs, such as Fe 36 C 108 O 156 ), dual-metallic organic frameworks (d-MOFs, such as Fe 26 Co 10 C 108 O 156 , Fe 30 Ni 6 C 108 O 156 ), and tri-metallic organic frameworks (t-MOFs, such as Fe 26 Ni 2 Co 8 C 108 O 156 ) for electrocatalytic OER. The DFT calculation and experimental results suggest that the OER performance could be promoted with reduced activation energy barrier and accelerated kinetics by introducing Co and Ni into the unit cell of Material of Institute Lavioisier (MIL). The optimized t-MOFs exhibited an ultra-low overpotential of only 200 mV at the current density of 10 mA cm −2 and a small Tafel slope of 34 mV dec −1 . This work proposes that the t-MOFs induced multi-metallic active sites and synergetic effect are promising strategies in designing highly efficient and robust OER electrocatalysts.
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