Advanced Healthcare Materials
·
2021
·Vol. 10
·期 19
·2100780
·
IF 9.933
Xin Meng,Fan Zhang,Huanling Guo,Chunyang Zhang,Hangtong Hu,Wei Wang,Jie Liu,Xintao Shuai,Zhong Cao
Smart theragnostic nanoplatforms exhibit great promise in clinical tumor treatment. The Fe-based Fenton reaction in tumor sites may generate reactive oxygen species to kill cancer cells with negligible side effects on normal tissues. However, its efficiency and duration are limited by the low intracellular concentration of H 2 O 2 , weak acidicity of tumor tissue, and low catalytic activity of conventional Fenton reagents. Herein, a facile strategy is proposed to efficiently overcome these obstacles. An efficient enzymatic/Fenton-starvation nanoreactor PMs loaded with glucose oxidase and perfluoropentane (PGPMs) is constructed through synthesizing methoxy-PEG-carboxymethy-modified iron (Fe 2+ /Fe 3+ )-based metal–organic frameworks (PMs), followed by loading glucose oxidase (GOx) and perfluoropentane (PFP). PGPMs accumulating in the tumor tissue exhibit tumor microenvironment-responsive biodegradable behavior and unusual catalytic activity for Fenton reaction advantageous over Fe 3+ -based MOFs. Meanwhile, encapsulation of GOx into PGPMs further significantly increases the catalytic activity for Fenton reaction and also induces starvation therapy. PGPMs also exhibit considerable capabilities of ultrasound and tumor microenvironment-responsive T2 MR imaging applicable for contrast-enhanced diagnosis. Both in vitro and in vivo studies demonstrate the great diagnostic and therapeutic potentials of this nanoreactor in tumor.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
·
材料科学
·
诊断成像
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhen Wang,Ying Fang,Ying Yang,Bo Qiu,Haipu Li
A rational design of high-performance catalysts with peroxymonosulfate (PMS) activation and arsenic adsorption capacities for the removal of p -arsanilic acid ( p -ASA) is in high demand but remains a significant challenge. Herein, vacancies-rich metal–organic frameworks (MOFs) were constructed by room-temperature co-precipitation procedure, and the magnetic CoFe encapsulated in N -doped carbon nanotubes (CoFe- N -CNTs) were prepared using MOFs template by an annealing process under a nitrogen atmosphere. The synthesis conditions of CoFe- N -CNTs were optimized by tuning Fe/Co ratio and carbonization temperature. The CoFe- N -CNTs/PMS system showed favorable removal performance, achieving complete degradation of 46 μM p -ASA within 3 min and a total arsenic removal efficiency of 98% within 30 min at 0.1 g/L catalyst and 400 μM PMS. The degradation rate ( k obs ) and total arsenic removal efficiency towards p -ASA by CoFe- N -CNTs/PMS system were 6.7 and 2.7 times of those in the MOFs without vacancies-derived catalyst/PMS system, respectively. CoFe- N -CNTs/PMS system exhibited robust and efficient performance over a broad range of pH (4.5–9.0) and in different water matrices. Scavenging experiments and electron paramagnetic resonance (EPR) results demonstrated that non-radical singlet oxygen ( 1 O 2 ), sulfate radicals (SO 4 − ), hydroxyl radicals ( OH), and superoxide (O 2 − ) were involved in p -ASA decomposition. Electron transfer and direct oxidative transfer process (DOTP) also contributed to p -ASA degradation. High-performance liquid chromatography coupled with inductively coupled plasma mass spectrometry (HPLC-ICP-MS) analysis indicated that the arsenic moiety was cleaved from p -ASA in the form of As(III) and then rapidly oxidized to As(V). X-ray photoelectron spectroscopy (XPS) analysis indicated the removal of inorganic arsenic followed the mechanism of the inner-sphere complex. This study highlights the in-situ synthesis of CoFe- N -CNTs with outstanding activities for catalytic degradation and arsenic removal of organoarsenicals.
研究领域:
环境科学
·
催化材料
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yang Wang,Shuaishuai Li,Chen Hou,Liming Jing,Rongkai Ren,Liweng Ma,Xu Wang,Jianzhi Wang
A biomass-based carbon fiber/metal–organic frameworks (MOFs/CF) electrode, with excellent electro-catalytic activity, was used for design the electro-Fenton (EF) process. The carbon fiber membrane (CF) was prepared from regenerated cotton fiber membrane through carbonization, and the MOFs were successfully introduced on the surface of the CF by the solvothermal method to obtain MOFs/CF electrode. Through the oxygen reduction reaction (ORR), the continuous on-site generation of H 2 O 2 was achieved over the MOFs/CF electrode. Moreover, the MOFs could efficiently catalyse H 2 O 2 to form hydroxyl radicals (•OH), which can degrade organic pollutants in the EF process. Excellent electrocatalytic performance was exhibited when the electrode was applied to degrade tetrabromobisphenol A (TBBPA). The total organic carbon removal efficiency for TBBPA reached 80% in 240 min, which demonstrated TBBPA was also rapidly mineralized by the constructed EF system.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Ximing Guo,Xueyao Tian,Xin Xu,Jinru He
In the manuscript, we developed a novel strategy to effectively improve the visible light absorption of Ti-based MOF by extending the conjugated degree of organic ligands in Ti-based MOFs. The freebased 5,10,15,20-tetraphenylporphyrin (H 2 TCPP) as organic linkers was used to facilely synthesize Ti-based MOFs (Ti-TiTCPP MOFs). The structural, morphologic and optical properties of Ti-TiTCPP MOFs were investigated. Ti-TiTCPP MOFs was applied to photocatalytic degradation of rhodamine B(RhB) and the photocatalytic degradation performances of Ti-TiTCPP MOFs were compared with that of NH 2 -MIL-125(Ti) MOFs under mercury lamp , xenon lamp and daylight lamp irradiation, respectively. The results showed the photocatalytic degradation performances of Ti-TiTCPP MOFs are superior to that of NH 2 -MIL-125(Ti) MOFs in visible region. Furthermore, the photocatalytic degradation mechanism of Ti-TiTCPP MOFs was investigated in detail based on the electrochemical and photoelectrochemical results associated with previously reported photocatalytic degradation mechanisms of NH 2 -MIL-125(Ti). The possible electrochemical and photoelectrochemical reactions and the changes of Gibbs free energy were analyzed. The degradation possible pathways of RhB and the emerging main intermediate contaminants were carefully analyzed by HPLC-HRMS under the present different solution parameters. And then the photocatalytic system based on Ti-TiTCPP MOFs was successfully applied to deal with real industrial textile wastewaters.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ying Zhang,Jiabin Zhou,Xin Chen,Luo Wang,Weiquan Cai
In this work, a Fe-based metal organic frameworks (MIL-88A) has been synthesized through a hydrothermal method and adopted as a high-efficiency catalyst for photocatalysis (PC) coupled with sulfate radical-based advanced oxidation processes (SR-AOPs) to degrade tetracycline hydrochloride (TC-HCl) under visible light irradiation. The effects of MIL-88A/persulfate (PS) molar ratio, initial solution pH and catalyst dosage were studied. The results indicated that the combining of the photocatalysis and SR-AOPs could remarkably enhance TC degradation and 200 mg/L 100 mL TC could be degraded completely at 0.25 g/L MIL-88A, unadjusted pH value and 4 mM PS in 80 mins. The results of scavenging experiments and ESR analysis demonstrated that SO 4 − • and •O 2– radicals were the predominant radicals for the TC degradation. The significant improvement of degradation rate in MIL-88A/PS/Vis process is attributed to the following two factors: (1) as a photocatalyst, MIL-88A could be excited by visible light, therefore photogenerated electrons (e − ) on the conduction band (CB) of MIL-88A could be trapped by PS to generate SO 4 − • radicals. In this process, PS acted as an electron acceptor and the electron/hole recombination was suppressed leading to the enhanced photocatalyst efficiency; (2) The PS can be activated not only by photoelectrons but also Fe (III) in MIL-88A leads to the generation of SO 4 − • radicals more rapidly and easily. A possible mechanism and degradation pathway for TC was proposed based on the trapping/ESR experiments and liquid chromatography-mass spectrometry (LC-MS) analysis. This work proposed a new idea and method in combining two oxidation processes in degradation of organic pollutants thus could be potentially used in environmental purification.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chunfeng Mao,Kai Yin,Chenghan Yang,Guomeng Dong,Guokai Tian,Yiwei Zhang,Yuming Zhou
Controlling the spatial confinement effect and highly dispersed Pd nanoparticles (NPs) can help to improve applicability in catalysis, energy conversion, and separation. However, the nonspatial confinement effect, agglomeration of Pd NPs of catalyst and harsh reaction conditions have become the urgent problems to be solved in Suzuki-Miyaura cross-coupling reaction. Herein, we report the first application of a new MOFs@COFs by using core with metal organic frameworks (MOFs) NH 2 -MIL-101(Fe) and shell with covalent organic frameworks (COFs) for loading Pd NPs. The quickly formation of a transition state, the highly dispersed Pd NPs and the advancedly spatial confinement effect were achieved by coupling Fe base synergistic active components, electron-oriented anchoring with controlling pore scale, respectively. Most notably, as a proof-of-concept application, the high catalytic activity of NH 2 -MIL-101(Fe)@Pd@COFs( 3 + 3 ) in catalysis is elucidated for Suzuki-Miyaura coupling reaction by the broad scope of the reactants and the preeminent yields of the products, together with excellent stability and recoverability. With this strategy, the mechanism of Suzuki-Miyaura coupling reaction was verified by examining the catalytic activity. We hope that our approach can further facilitate the study of the design and use of functional MOFs@Pd@COFs materials.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Aotian Gu,Kaiwei Chen,Xinyu Zhou,Chunhui Gong,Peng Wang,Yan Jiao,Ping Mao,Kai Chen,Jigen Lu,Yi Yang
Advanced oxidation processes based on high-valent metal species have attracted much attention due to their high reactivity and selectivity in degrading refractory organic pollutants, but the preparation of such catalysts remains a great challenge. Herein, FeCoCu-nitrogen-doped carbon (FeCoCu-NC), a trimetallic catalyst capable of producing high-valent metal species, was synthesized by direct carbonization of core–shell Metal-organic frameworks (MOFs). The rationally designed catalyst exhibited high catalytic activity in wide pH range and high resistance to common radical scavengers, anions and natural organics. The incorporation of Cu in FeCoCu-NC (TNC X ) not only enhanced the catalytic activity but also changed the activation mechanism of peroxymonosulfate (PMS) from a radical pathway to a non-radical pathway dominated by high-valent metal species. In addition, the TNC 5 /PMS system showed higher trichlorophenol (TCP) removal efficiency and PMS utilization compared to the radical-dominated FeCo-NC/PMS system and the 1 O 2 -dominated CoCu-NC/PMS system. This study provides a facile strategy to the preparation of advanced catalysts from multi-metal MOFs and is expected to provide guidance for the design of heterogeneous high-valent metal catalysts.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Advanced Research
·
2020
·
IF 6.992
Tengfei Li,Meng Lu,Yuhang Gao,Xiaodong Huang,Guangyang Liu,Donghui Xu
In this study, a novel metal-organic framework (M-ZIF-8@ZIF-67) was successfully prepared using the single layer Fe 3 O 4 -ZIF-8 as magnetic core and wrapped a layer of ZIF-67 outer. This M-ZIF-8@ZIF-67 was employed as an adsorbent for the adsorption and removal of fipronil and its metabolites from environmental water and cucumber samples. The characterization results suggested that M-ZIF-8@ZIF-67 has the double layer structure a polyhedral structure with uniform pores, while ZIF-67 was successfully coated on the surface of Fe 3 O 4 -ZIF-8. The unique structure endowed M-ZIF-8@ZIF-67 a high surface area (219 m 2 /g) and high adsorption capacity for fipronil, fipronil desulfinyl, fipronil sulfide and fipronil sulfone. To our knowledge, this is the first report detailing the adsorption properties of M-ZIF-8@ZIF-67 with double layer structure relating to the adsorption and removal of pesticides. Furthermore, the adsorption model analysis demonstrated that the static adsorption data fitted the Freundlich bimolecular layer adsorption model better than the Langmuir monolayer adsorption model. This study indicates that M-ZIF-8@ZIF-67 has significant potential in the adsorption and removal of fipronil and its metabolites in water and vegetable samples.
研究领域:
环境科学
·
材料科学
·
农业科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Chunhua Li,Zhehang Tian,Guanqun Luan,Luqian Bao,Mengyao Cui,Yixin Ji,Xieyang Zhang
The extensive use of tetracyclines in livestock poses health risks due to their residues in animal-derived food; therefore, developing simple detection methods to replace complex traditional approaches is of paramount importance. Here, we developed a dual-ligand zinc-based metal–organic framework material, Zn-BTC-BDC-NH2 (denoted as ZTD), for the detection of tetracyclines. The intrinsic blue fluorescence of ZTD was quenched upon the introduction of tetracyclines due to electron transfer from −NH2 of ZTD to −CO– and −OH groups of tetracycline molecules; meanwhile, the new green fluorescence emission was generated through π–π stacking between aromatic rings and the formation of complexes between Zn2+ and C–O/C═O groups. In real food samples, ZTD exhibited recovery rates ranging from 93.62 to 110.66%, with detection limits as low as 0.011 μmol·L–1. Additionally, a ZTD fluorescence test paper was developed for portable detection. This study presents a novel tetracycline detection method, offering insights into multiligand metal–organic framework preparation and future sensing method design.
研究领域:
材料科学
·
食品安全
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Cuizhu Ye,Xingguang Chen,Junjun Xu,Huiting Xi,Tiantian Wu,Danwen Deng,Jinsheng Zhang,Ganhui Huang
Supported by metal-organic frameworks (MOFs), a new molecular imprinted electrochemical sensor (MIES) taking nano-structure Co 2+ @Fe 3 O 4 as the support point of receptor was developed for highly sensitive detection of GA in this paper. Gold electrode was modified with Co 2+ @Fe 3 O 4 , then Co 2+ @Fe 3 O 4 /Au was soaked and compounded to Fe 3 O 4 @ZIF-67/Au. MIPs film was obtained by potentiostatic polymerization with polypyrrole as monomer and GA as template. SEM, EDS, FTIR, XRD, DPV and EIS characterizations indicate the success of the preparation of the modified electrode . By optimization, the Δ i response of MIP/Fe 3 O 4 @ZIF-67/Au was strengthened from 25.38 μA to 30.84 μA. The MIP/Fe 3 O 4 @ZIF-67/Au sensor showed a superior sensitivity with a lower LOD of 0.297pM (S/N = 3) and a wider linear range of 6–600pM for GA detection, which profits from the combination of high surface area of Co 2+ @Fe 3 O 4 and high porosity of MOFs. Because of the specificity of molecular imprinted polymers (MIPs), our sensor showed advanced selectivity and not affected by similar structure interfering substances. In addition, the stability, reproducibility and real-sample detection were also satisfactory with the recovery rates between 89.5% and 118.4% and the RSD were lower than 5.5%. This sensitive and simple method can be further used to prepare polypyrrole-based MIES suported by MOFs-Co 2+ @Fe 3 O 4 for highly sensitive detection of other small and weight molecules.
研究领域:
分析化学
·
电化学
·
纳米技术
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Qingtai Chen,Chongchong Wu,Shujie Hu,Lizhi Cui,Yong Zhang,Peng Hu,Zhi Xu,Pei Yu,Miao Yu
Xylanase is a natural and high-efficiency catalyst for the degradation of xylan to reducing sugar. However, the catalytic performance of xylanase is greatly limited by its poor activity and stability at the harsh condition. To overcome this issue, covalent immobilization of xylanase on a magnetic porous MOFs material with core-shell structure, UIO-66-NH2 carrier was applied to improve the catalytic activity and stability of xylanase. Several tools were employed to monitor the preparation and immobilization processes, magnetic properties, and the structural/chemical characteristics of the biocatalyst. 77.9% of the activity for xylanase was retained after immobilization. Moreover, the thermal stability in terms of half-life of the immobilized enzyme was three times higher than that in free form, and which had higher catalytic efficiency for hydrolysis of xylan. Furthermore, the greater temperature and wider pH ranges of the activity stability were achieved for the immobilized xylanase in compared with free one. Notably, the biocatalyst exhibits both excellent storage stability and could be easily separated using a magnet, which is conducive for its reusability. And nearly 70% of its initial activity was retained after seven recycles during the hydrolysis of corn straw. These features indicate that the present immobilization method is promising prospect for the industrial application of enzyme.
研究领域:
生物技术
·
酶工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Bin Cao,Mengyu Li,Ye Zhao,Huimin Zhou,Ting Tang,Mengran Li,Chuan Song,Wei Zhuang
In recent years, two-dimensional nanosheet metal-organic frameworks (2D MOFs) have been widely considered as promising carriers for enzyme immobilization owing to their large surface area, designable and tunable structures, and other properties that enhance enzyme loading and modulate interactions with enzymes. In this study, a series of ultrathin 2D M-TCPP (M = Co, Ni, Zn, Cu) nanosheets were synthesized employing a surfactant-assisted bottom-up approach, and the effect of solvent ratio on the morphology and properties of 2D MOFs was explored. After systematic characterization, Cu-based 2D MOFs with large specific surface areas and excellent water stability was selected as the carrier for the co-immobilization of glucose oxidase (GOx) and horseradish peroxidase (HRP). The effects of adsorption and covalent immobilization strategies on bis-enzyme loading and enzyme activity , as well as their applications in rapid glucose detection, were systematically investigated. The results showed that A-CTGH and C-CTGH owned enzyme loadings of 187.9 and 249.1 mg/g, respectively, and exhibited superior enzymatic activity when exposed to harsh environments compared to free enzymes. In addition, the covalently immobilized biocatalyst based on GOx demonstrated a more sensitive glucose detection performance, including a wide linear range from 5.0 to 16 μM with a detection limit of 0.6 μM.
研究领域:
纳米材料
·
生物催化
·
分析化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）