SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Zhi Hu,Shucheng Liu,Nana Tang,Xuan Zhang,Jianming Pan
The main obstacles of recognition of flavoniods are low concentration and complexity of extract wastewater solutions. The structural and stability limitation of the sorbents is the significant reason for the difficulty in increasing the adsorption amount in the separation system. Hereon, a novel hierarchical-pore boronic acid-functionalized-MOFs based on macroporous organo/hydro copolymers (CPs@H-UiO-66-NH 2 @BA) were firstly fabricated through the triple sacrificial cross-linking strategy, which allowed the formation of multiple hydrogen bond networks (i.e. main crosslinked networks and weak crosslinked networks) at oil–water interface. Noticeably, the MOFs with polymer chain entanglement effects as a physical sacrificial cross-linking network, significantly enhancing the mechanical properties. The maximum equilibrium binding capacity of CPs@H-UiO-66-NH 2 @BA was 40.93 µmol g −1 for NRG at 308 K. Furthermore, it also showed superior regeneration capacity capability (only 7.81% loss) after six cycles. Meanwhile, they had a stronger selectivity towards NRG. It can effectively purify the low purity of the actual sample ground to 92.68%. It is anticipated that in-situ the introduction of nanoboronic-functionalized MOFs construction into copolymers would hold great promise in the selective capture of target flavonoids in actual samples.
研究领域:
材料科学
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化学工程
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分析化学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 37
·14306-14316
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IF 4.569
Hao Wu,Qingxi Zhai,Fan Ding,Dongyue Sun,Yujie Ma,Yilun Ren,Biao Wang,Fengqi Li,Haifeng Bian,Yurong Yang,Lan Chen,Shaochun Tang,Xiangkang Meng
The preparation of low-cost and high-activity oxygen evolution reaction (OER) catalysts is a technical bottleneck in the field of electrolysis of water to produce hydrogen. Amorphous metal–organic frameworks (MOFs) with low-cost transition metals have attracted increasing attention in the catalytic field, yet metal atoms that are the main active sites are still ambiguous. Here, we synthesized a series of amorphous ternary Fex(NiCu)3−x-MOFs via an ultrasonic method. The optimal amorphous FeNiCu-MOF is found to be able to supply a current density of 10 mA cm−2 merely at a low overpotential of 260 mV with a small Tafel slope of 61 mV dec−1 and exhibits high durability over 24 h. Moreover, density functional theory (DFT) calculations show that the Fe atoms are the main active sites for the OER in the FeNiCu-MOF. This work shows that amorphous ternary MOFs have great potential for application in OER electrocatalysts due to the multiple synergistic effects and amorphous MOF structures.
研究领域:
材料科学
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电化学
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催化
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zheng Xiaomei,Lin Rujing,Xu Jun,He Yingying,Zhang Xinying,Xie Li
Cathode materials play important roles in the optimization of methane upgrading in microbial electrolysis cell-coupled anaerobic digestion (MEC-AD) systems. In this study, metal organic framework (MOF)-derived carbon-based bimetallic hybrids (Ni/Co-NC) was synthesized as cathode material and its performances and microbial activities were evaluated in MEC-AD. A high methane production rate (0.57 m 3 CH 4 /m 3 ·d) and yield (0.34 m 3 CH 4 /kgCOD) were achieved with a Ni/Co-NC cathode at a potential of 0.6 V. The methane content in the biogas was upgraded to ca. 90%. The enhanced methane production was likely related to the positive surface charge and the good conductive capacity and hydrogen evolution of the Ni/Co-NC cathode, as demonstrated by electrochemical assessment. Additionally, roughness and extensive surface areas provided additional room for cathodic biofilm adhesion via hydrogen bonding and electrostatic interactions. A significant enrichment of Methanobacterium (79.6%) in the MEC-AD-Ni/Co-NC system, especially in the biofilm of the cathode surface, indicated that the methane production pathway shifted from acetoclastic to hydrogenotrophic methanogenesis. Moreover, Methanosaeta harundinacea 6Ac species, which can directly accept electrons, were identified in the MEC-AD systems. These findings revealed that Ni/Co-NC cathode probably enhanced bioelectrochemical reduction of CO 2 to CH 4 by accelerating hydrogenotrophic methanogenesis and direct electron transfer.
研究领域:
环境工程
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微生物学
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电化学
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生物技术
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2018
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IF 3.235
Shuang Zhao,Yuchan Zhang,Songtao Ding,Jingchuan Fan,Zhi Luo,Kunguo Liu,Qi Shi,Weichi Liu,Guangchao Zang
A reliable and non-invasive electrochemical immunosensor for nuclear matrix protein 22 (NMP22) was presented based on reduced graphene oxide-tetraethylenepentamine (rGO-TEPA) and gold nanoparticles‑platinum nanoparticles-metal organic frameworks (AuNPs-PtNPs-MOFs) nanomaterial . rGO-TEPA is a promising template to enhance the loading ability of electrode for its large specific surface area and abundance in amino groups. AuNPs-PtNPs-MOFs nanomaterial was synthesized by NaBH 4 reduction method and applied to immobilize biomolecules due to their good biocompatibility, well conductivity , and excellent H 2 O 2 electrocatalytic ability. The electrochemical response signal was primarily originated from the obstruction of immobilized NMP22 antigen towards electrocatalytic reduction of H 2 O 2 and the signal was recorded by differential pulse voltammetry . Under optimum conditions, the immunosensor showed a sensitive response towards NMP22 at a broad concentration range from 0.005 ng·mL −1 to 20 ng·mL −1 . Two strong linear ranges could be observed at 0.005 ng·mL −1 to 0.5 ng·mL −1 (R 2 = 0.9833), and 0.5 ng·mL −1 to 20 ng·mL −1 (R 2 = 0.9909), with a low LOD of 1.7 pg·mL −1 (S/N = 3). Satisfactory reproducibility, stability and selectivity were obtained for NMP22 detection in real urine samples compared with standard ELISA assay, demonstrating the good analytical performance and potential non-invasive clinical application of this label-free electrochemical immunosensor.
研究领域:
分析化学
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生物传感器
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纳米技术
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医学诊断
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Liangdi Jiang,Zhouyang Huang,Jiacan Xu,Liqiu Zhang,Ziwen Du
Selectivity is the key for adsorption or recovery of per- and polyfluoroalkyl substances (PFAS) from aqueous environments. In this study, the fluorinated metal–organic frameworks (MOFs) with different fluorine contents were prepared and investigated to evaluate the selective adsorption of an emerging PFAS, sodium p‑perfluorous nonenoxybenzenesulfonate (OBS). Adsorption of OBS increased with the increasing fluorine content of MOFs, and the best fluorinated MOFs showed an excellent selective adsorption capacity. The influence of various co-existing hydrocarbon substances on OBS adsorption was slight. The adsorption amount of OBS was 15-fold to that of the hydrocarbon surfactants (n-caprylic acid). The selectivity was attributed to the fluorinated structures of MOFs whose oil contact angle was up to 101°, and thus the oleophobicity of fluorinated structures made MOFs repel hydrocarbon compounds. Molecular dynamics simulations and density functional theory calculations indicated that the fluorinated structures were able to capture OBS molecules from the long distances (roughly 1–100 nm) via hydrophobic interaction, and then formed a F–F non-covalent interaction which was highly probable to be driven by a dispersion force to further attract OBS fluorinated tails within shorter distances (less than 3.5 Å). The combination of oleophobic and fluorophilic effects contribute to the exclusive selectivity of fluorinated MOFs for OBS molecule.
研究领域:
环境科学
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材料科学
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化学
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产品关联
DOI
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Weizuo Li,Jing Wang,Dafang He,Guangyu He,Haiqun Chen
Developing highly efficient MOFs derived alloy catalysts for the one-pot tandem catalytic reactions remains a challenge. In this work, a novel solid-solution confined NiCo alloy catalyst incorporating carbon (termed as NiCo/MgO-C) with banana-like morphology has been synthesized via a self-templating strategy for directing pyrolysis of well-defined Ni-Co-Mg tri-metallic MOFs (termed as Ni-Co-Mg@H 2 dhbdc, H 2 dhbdc represents 2,5-dihydroxytelephthalic acid organic linker). The developed NiCo/MgO-C catalyst was applied for the hydrogenation-alkylation tandem catalytic reaction. Owing to the unique structural (e.g., highly dispersed, small size of NiCo nanoparticles, enhanced transfer of electron density) as well as NiCo alloy advantages, the developed NiCo/MgO-C catalyst derived from Ni-Co-Mg@H 2 dhbdc MOFs delivers excellent superior catalytic performance for the hydrogenation-alkylation tandem reaction to those of bimetallic MOFs (Ni-Mg@H 2 dhbdc and Co-Mg@H 2 dhbdc, respectively) derived catalysts (Ni/MgO-C and Co/MgO-C, respectively). Notably, the tri-metallic Ni-Co-Mg@H 2 dhbdc served as the precursor for synthesis of developed catalyst could enhance the reduction degree of NiO/CoO species confined in NiO CoO-MgO solid-solution during the pyrolysis process to some extent. Therefore, we anticipated that this tri-metallic MOFs-templated strategy may provide a facile and controllable way for synthesis of solid-solution supported nanoalloy catalysts for the other heterogeneous catalytic reactions.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
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2021
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IF 9.811
Ke Li,Jian Yang,Jinlou Gu
The creation of artificial microenvironments with specific functionalities to mimic multiple cascade biocatalytic processes in cells is highly desirable. Here, Zr-based large-pore mesoporous metal–organic frameworks (mesoMOFs) were successfully developed for the construction of such spatially organized cascade bioreactors. Thanks to the mediating effect of the Hofmeister ion and the flexibility of Zr-MOFs, large mesopores and functional microporous mesopore walls were integrated into a single nanoplatform, ensuring the efficient mass exchange between the interconnected pore units with different sizes. As a proof of concept, natural superoxide dismutase and catalase mimic were spatially positioned in these hierarchical mesoMOFs, which formed a cascade antioxidant defense system and presented an efficient intracellular reactive oxygen species scavenging ability. This model is expected to set a conceptual guideline for the design of compartmentalized bioreactors in nanoscale MOFs to mediate the complex intracellular catalytic networks.
研究领域:
纳米技术
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生物催化
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材料科学
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生物化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yanyan Ji,Wenjing Li,Weiping Cao,Zhen Yang,Chunming Zheng,Wu Zhang
In this work, Cu-Fe bimetal-embedded carbonaceous CuFe@C materials were prepared by high-temperature pyrolysis of CuFe-MOFs precursors synthesized through a facile two-step feeding approach. Through adjusting the reaction time of each feeding step, CuFe-MOFs of uniform dispersed crystals with controlled sizes were obtained. The carbonized composites were then applied to activate persulfate (PMS) for Reactive Brilliant Red X-3B (RBRX-3B) degradation in water. The removal rate of RBRX-3B was up to 98% in 40 min in the CuFe@C 600 /PMS system, indicating that the CuFe@C 600 catalyst showed excellent sulfate radical-based oxidation (SR-AO) activity in the degradation process. The effects of PMS dosage, initial pH, RBRX-3B concentration on the degradation efficiency were investigated in detail. Based on quenching experiments, a possible mechanism for the CuFe@C 600 /PMS system was proposed. The catalyst had good reusability, in which the removal rate of RBRX-3B could attain 82% after 5 times of repeated recycling. It also showed satisfactory removal effect on other organic pollutants, i.e. Congo red, Methyl orange, Reactive blue and p-nitrophenol. This study provided a valuable strategy for the treatment of wastewater containing organic pollutants using MOFs-derived materials.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Yue Wang,Hongguo Zhai,Qi Guo,Yuhao Zhang,Xia Sun,Yemin Guo,Qingqing Yang,Yanyan Zhang
Heavy metals and foodborne pathogens have become key pollutants that harm aquatic products, seriously endangering food safety and human health. Therefore, in this study, a ratiometric electrochemical aptamer sensor with a novel signal amplification strategy was constructed using ZrO 2 as the substrate and Ni/Co-MOFs@AuNPs cubic nanomaterials to increase the specific surface area to simultaneously detect Cd 2+ and S.aureus. The shared hairpin complementary chains modified with ferropene (Fc) could simultaneously bind to the Cd 2+ and S.aureus aptamers modified with methylene blue (MB) and anthrquinone-2-carboxylic acid (AQ). The ratios of MB and AQ to Fc were used to realize the qualitative and quantitative detection of Cd 2+ and S.aureus. Under the optimal conditions, the electrochemical aptamer sensor for Cd 2+ and S.aureus was in the range of 1.00 × 10 −2 -1.00 × 10 4 ng/L and 1.00 × 10 1 -1.00 × 10 7 CFU/mL, and the lowest detection limit was 1.91 × 10 −4 ng/L and 1.37 CFU/mL, respectively. The aptasensor constructed in this paper can realize the simultaneous detection of Cd 2+ and S.aureus in scallop and fish, providing a new detection method for the simultaneous detection of a variety of aquatic products pollutants.
研究领域:
分析化学
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环境科学
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食品科学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Lei Li,Hengji Liu,Yuanyuan Wang,Gang Wang,Yongde Guo,Weimin Kang
Reasonable construction of low migration energy barrier and continuous proton transfer channel is the key to improving the performance of composite proton exchange membranes. In this paper, we prepared a novel bimetallic MOFs (MIL-(Cr Al)–NH 2 ) nanofibers (MCANs) consisting of Cr and Al elements by electro-blown spinning method (EBS) and hydrothermal synthesis, and subsequently introduced them into non-fluorinated sulfonic acid polymer sulfonated polysulfone (SPSF) matrix to obtain composite proton exchange membranes (MCANs@SPSF). Importantly, MCANs successfully constructed relatively long-range continuous unsaturated metal site proton transfer channels provided by the Cr-based MOFs, thereby reducing the proton migration energy barrier in the MCANs@SPSF, which confirmed by the density functional theory (DFT) calculation. In detail, DFT studies indicated that the migration energy barrier between H + and MCANs was 1.677 eV, while that of single Al-based MOF (MAN) and single Cr-based MOF (MCN) were 1.879 eV and 1.762 eV respectively. The existence of efficient low migration energy barrier and continuous proton transfer channels made the proton conduction efficiency of MCANs@SPSF greatly improved, that was under the condition of 80 °C and 100 % RH, the proton conductivity of MCANs@SPSF reached the maximum value of 0.358 S cm −1 and the power density reached 104 mW cm −2 . Moreover, MCANs@SPSF-5 displayed best DMFC durability performance with only 14.65 % voltage loss under 24h test. In addition, due to the acid-base pair interaction between MCANs and SPSF enhanced the interface binding force between the two phases, meanwhile, the pore structure of MOFs also had a certain adsorption effect on methanol, thus reducing the methanol permeability, and the addition of 5 wt% MCANs in SPSF was tested to reduce the methanol permeability to 5.53 × 10 -7 cm 2 s −1 . Overall, this work provided a new strategy for construction of low migration energy barrier and continuous proton transfer channels, which was beneficial for the development of high performance proton exchange membranes.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shuhong Huang,Yan Wang,Shuying Qiu,Jinquan Wan,Yongwen Ma,Zhicheng Yan,Quanmo Xie
Since high degradation efficiency and environmental friendliness, the Electro-Fenton technology has been widely applied to remove antibiotics in wastewater. In-situ loading of electrochemically active metals on graphite felt (GF) is considered as a promising strategy for improving its electrocatalytic activity and reusability. Here, a series of Mn/Co MOFs derivatives modified graphite felt cathodes (Mn x Co 3-x @C-GF) were fabricated without any binder, which was used for the treatment of ciprofloxacin (CIP). The morphology, pore structure and electrochemical activity of Mn x Co 3-x @C-GF changed by adjusting the ratio of Mn/Co in the MOF-74 precursor. Owning to the optimized Mn/Co ratio, Mn 2 Co 1 @C-GF exhibited the most excellent catalytic ability with hierarchical porous structure and faster electron transfer . The results showed that the CIP degradation efficiency could reach 99.8% in 60 min. Mn 2+/3+/4+ and Co 3+/2+ enhanced the generation of active radicals (·OH) by Fenton-like reaction and further improved degradation performance. In addition, the cathode had maintained good stability during four cycles. This work provides an alternative strategy for fabricating efficient self-supporting cathode materials in the future.
研究领域:
环境科学
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化学工程
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材料科学
·
水处理
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Jiabin Zhang,Kai Wang,Shiyao Xu,Linlin Chen,Haiquan Gu,Yujie Yang,Qi Zhao,Yurou Huo,Bo Li,Yufei Wang,Yubiao Xie,Nan Li,Jiali Zhang,Jianxu Zhang,Qianxue Li
Vaccines are widely regarded as one of the most effective weapons in the fight against infectious diseases. Currently, vaccines must be stored and transported at low temperatures as high temperatures can lead to a loss of vaccine conformation and reduced therapeutic efficacy. Metal–organic frameworks (MOFs), such as zeolitic imidazole framework-8 (ZIF-8), are a new class of hybrid materials with large specific surface areas, high loading rates, and good biocompatibility and are successful systems for vaccine delivery and protection. Silk fibroin (SF) has a good biocompatibility and thermal stability. In this study, the hepatitis B surface antigen (HBsAg) was successfully encapsulated in ZIF-8 to form HBsAg@ZIF-8 (HZ) using a one-step shake and one-pot shake method. Subsequently, the SF coating modifies HZ through hydrophobic interactions to form HBsAg/SF@ZIF-8 (HSZ), which enhanced the thermal stability and immunogenicity of HBsAg. Compared to free HBsAg, HZ and HSZ improved the thermostability of HBsAg, promoted the antigen uptake and lysosomal escape, stimulated dendritic cell maturation and cytokine secretion, formed an antigen reservoir to promote antibody production, and activated CD4+ T and CD8+ T cells to enhance memory T-cell production. Importantly, HSZ induced a strong immune response even after 14 days of storage at 25 °C. Furthermore, the nanoparticles prepared by the one-step shake method exhibited superior properties compared to those prepared by the one-pot shake method. This study highlights the importance of SF-coated ZIF-8, which holds promise for investigating thermostable vaccines and breaking the vaccine cold chain.
研究领域:
药学
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纳米技术
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免疫学
·
疫苗开发
✓ 已验证
DOI
PubMed
高影响因子