TALANTA
·
2021
·
IF 6.057
Xuemin Huang,Qingfeng Liu,Cuimin Wu,Zhenyu Lin,Aiwen Huang,Bin Qiu
As a popular controllable-released carrier, intelligent hydrogels are often used in drug delivery and disease therapeutics. Meanwhile, benefit from the mimic-enzyme activity performance, Fe–N–C nanozymes have been widely used in sensing and analysis. However, the combination of intelligent hydrogels with specific degradability and Fe–N–C nanozymes with enhanced activity in one system to achieve controllable and sensitive detection is rare. Herein, we combine intelligent hydrogel with mimic peroxidase activity enhanced Fe–N–C nanozymes to construct a ratiometric fluorescence probe for sensitive detection of hyaluronidase (HAase). The modification of copper ions has been proved to enhance the mimic enzyme activity of Fe–N–C nanozymes greatly. Cu 2+ modified Fe–N–C nanozymes were embedded in hyaluronic acid hydrogel. In the presence of HAase, the HA hydrogel structure was hydrolyzed and released Cu 2+ -Fe-N-C nanozymes gradually. The released Cu 2+ -Fe-N-C nanozymes are used to catalyze the hydrogen peroxide system so that o-phenylenediamine is oxidized to orange fluorescent 2, 3-diaminophenolazine (DAP). Due to the electrostatic interaction , the fluorescence resonance energy transfer can occur between the negatively charged copper nanoclusters emitted by 430 nm and the positively charged DAP emitted by 560 nm. The activity of HAase was monitored according to the ratio of fluorescence intensity at 560 nm and 430 nm (F560/F430). The linear range of this method is 0–10.0 U/ml and the detection limit is 0.43 U/mL (S/N = 3). This strategy has been further applied to biological samples successfully.
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Nano Research
·
2020
·Vol. 13
·期 1
·273-281
·
IF 8.183
Zhang Tao,Jiang Zhenqi,Chen Libin,Pan Chunshu,Sun Shan,Liu Chuang,Li Zihou,Ren Wenzhi,Wu Aiguo,Huang Pintong
As nanomedicine-based clinical strategies have continued to develop, the possibility of combining chemotherapy and singlet oxygen-dependent photodynamic therapy (PDT) to treat pancreatic cancer (PaC) has emerged as a viable therapeutic modality. The efficacy of such an approach, however, is likely to be constrained by the mechanisms of drug release and tumor oxygen levels. In the present study, we developed an Fe(III)-complexed porous coordination network (PCN) which we then used to encapsulate PTX (PCN-Fe(III)-PTX) nanoparticles (NPs) in order to treat PaC via a combination of chemotherapy and PDT. The resultant NPs were able to release drug in response to both laser irradiation and pH changes to promote drug accumulation within tumors. Furthermore, through a Fe(III)-based Fenton-like reaction these NPs were able to convert H 2 O 2 in the tumor site to O 2 , thereby regulating local hypoxic conditions and enhancing the efficacy of PDT approaches. Also these NPs were suitable for use as a T 1 -MRI weighted contrast agent, making them viable for monitoring therapeutic efficacy upon treatment. Our results in both cell line and animal models of PaC suggest that these NPs represent an ideal agent for mediating effective MRI-guided chemotherapy-PDT, giving them great promise for the clinical treatment of PaC.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Zhen Song,Yang Li,He Teng,Caifeng Ding,Guiyun Xu,Xiliang Luo
Herein, an antifouling and sensitive electrochemical enzyme sensing platform was developed based on a self-designed zwitterionic peptide and sacrificial iron metal-organic framework (Fe-MOF). The designed zwitterionic peptide was hydrophilic and neutral in charge, and it was used to improve the antifouling capability of the sensing system. Fe-MOF with amine groups was loaded with Au nanoparticles and further functionalized with a specific DNA sequence, and it was used as a sacrificial label. The sensing target, T4 polynucleotide kinase (PNK), can catalyze the 5′-hydroxyl termini of a unique hairpin DNA to phosphate group, and the hairpin DNA can then be hydrolyzed by lambda exonuclease (λ-Exo) and release a single nucleotide. In the presence of the released DNA sequence, a sandwich-type hybridization reaction was triggered, and the DNA linked Fe-MOF was selectively attached to the electrode surface, which can react with K 4 Fe(CN) 6 to form the electroactive Prussian blue and generate significantly enlarged current response. Based on the antifouling peptide and the sacrificial Fe-MOF, the biosensor exhibited satisfying analytical performance for the detection of T4 PNK, with a wide linear range from 1.0×10 −3 to 10 U·mL -1 and a low detection limit of 3.5×10 -4 U·mL -1 . Moreover, the biosensor was capable of effectively eliminating nonspecific protein adsorption and assaying target in human serum, indicating its promising potential for practical application.
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ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Lihua Gao,Zhenggen Liu,Yuzhu Pan,Cong Feng,Yang Ge,Mansheng Chu
Carbothermal reduction followed by magnetic separation has been recognized as an effective recovery strategy to achieve separation of Mn and Fe from ferruginous manganese ores (Fe-Mn ores). However, it is difficult to improve the recovery of manganese more than 85% by changing carbothermic roasting reduction and magnetic separation. This work clarified the underlying reason for the poor separation with the magnetic separation process and proposed a promising process for the recovery of Fe and Mn from Fe-Mn ore. The effect of operating variables on recovery and separation of Mn and Fe from Fe-Mn ore is initially investigated during the carbothermic reduction roasting process followed by magnetic separation to reveal the underlying reason for the poor separation from Fe-Mn ores. Then, the stepwise reduction behaviors of the MnO-Fe 2 O 3 and MnO-Fe 2 O 3 -Al 2 O 3 systems were investigated to clarify that the formation of composite oxide Mn 1−x Fe x O (0 < x < 0.497) and hercynite (FeO·Al 2 O 3 ) directly caused the poor separation of Fe and Mn from high-alumina Fe-Mn ores. Then, the stepwise reduction roasting behaviors of Mn 1−x Fe x O and FeO·Al 2 O 3 were investigated by XRD, SEM-EDS and XPS analysis. After adjusting the experimental parameters, iron-rich products with a Fe recovery of 94.31% and a grade of 85.21% and manganese-rich product with a Mn recovery of 90.05% and a grade of 54.35% are obtained. The mass ratio of Mn/Fe increased to 8.5 in the manganese-rich product.
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ENVIRONMENTAL RESEARCH
·
2019
·
IF 5.026
Ying Li,Yijie Han,Wei Li,Yuxin Li,Deyun Zhang,Yeqing Lan
A novel magnetic sulfur-doped Fe–Cu–Y trimetal oxide (MST) nanomaterial was successfully synthesized by a chemical coprecipitation method to remove As(III) via simultaneous oxidation and adsorption and then characterized by BET, VSM, FESEM, XPS, and FTIR techniques. The effect of solution initial pH on the adsorption of As(III), and the adsorption kinetics and isotherm were investigated in detail. The results indicated that the MST nanoparticles exhibited an excellent performance for As(III) removal in a pH range of 7–10 and were easily separated from aqueous solution with a magnet. The maximum removal capability for As(III) reached 202.0 mg/g at pH 7.0. The adsorption of As(III) was well fitted by the pseudo-second-order kinetic model and Langmuir isotherm model, respectively. The investigation of mechanism revealed that As(III) could be oxidized to As(V) by O 2 − and OH free radicals, generated via the dissolved O 2 obtaining an electron from Cu(I) on the surface of the adsorbent and Fenton/Fenton-like reaction, respectively. Meanwhile, the produced As(V) was adsorbed onto the surface of the nanoparticles through the electrostatic attraction or diffusion. The adsorbed As(V) further interacted with –OH groups via ion exchange or with Y(III) on the surface of the adsorbent to form a precipitate. Therefore, the MST nanoparticles are promising for the removal of arsenic from water.
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Nanomaterials
·
2019
·Vol. 9
·期 2
·E210
·
IF 4.034
Qingtong Zhang,Mingfu Li,Chenyan Guo,Zhuan Jia,Guangcong Wan,Shuangfei Wang,Douyong Min
Lignin is the second largest naturally renewable resource and is primarily a by-product of the pulp and paper industry; however, its inefficient use presents a challenge. In this work, Fe₃O₄ nanoparticles loaded on lignin nanoparticles (Fe₃O₄@LNPs) were prepared by the self-assembly method and it possessed an enhanced peroxidase-like activity. Fe₃O₄@LNPs catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H₂O₂ to generate a blue color, was observable by the naked eye. Under the optimal conditions, Fe₃O₄@LNPs showed the ability of sensitive colorimetric detection of H₂O₂within a range of 5⁻100 μM and the limit of detection was 2 μM. The high catalytic activity of Fe₃O₄@LNPs allows its prospective use in a wide variety of applications, including clinical diagnosis, food safety, and environmental monitoring.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Sijia Li,Jianan Cui,Xia Wu,Xuan Zhang,Qi Hu,Xiaohong Hou
Metal-Organic Frameworks (MOFs) are efficient adsorbent and catalyst, however, the prepare of MOFs can be extremely time consuming. The rapid in situ microwave synthesis process offers the possibility of MOFs to a large-scale application. In this study, Fe 3 O 4 @MIL-100(Fe) was rapidly prepared via microwave in 30 min using Fe 3 O 4 as metal precursor and applied as the adsorbent and photocatalyst to remove diclofenac sodium (DCF) from water. Fe 3 O 4 @MIL-100(Fe) exhibited an excellent adsorption effect to DCF with the maximum adsorption capacities of 400 mg/L. The presence of H 2 O 2 could promote the removal of DCF during photocatalytic process. Approximately 99.4% of the DCF was removed in Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 system via adsorption removal and consequent photocatalytic degradation . The high efficiency was attributed to the large BET surface area (1244.62 m 2 /g) and abundant iron metal sites (Fe(III) and Fe(II)) of Fe 3 O 4 @MIL-100(Fe). The adsorptive, photocatalytic property of Fe 3 O 4 @MIL-100(Fe) and the Fenton-like reaction were the main mechanisms for DCF removal. TOC analyzer was served to assess the mineralization of solutions treated by Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 in 12 h. High elimination of TOC (87.8%) was observed during the DCF mineralization process. In addition, the major products were illuminated using HPLC-Q-TOF-MS and DCF degradation pathways were also proposed.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Rongfa Ding,Hui Wang,Yan Jiang,Rui Liu,Ke Jing,Meng Sun,Ruiqian Zhang,Shaoyu Qiu,Zhuoming Xie,Haowei Deng,Xianping Wang,Mingguang Kong,Weibin Jiang,Qianfeng Fang,Changsong Liu
ZrC dispersion-strengthened FeCrAl alloys with enhanced high-temperature strength and good ductility were fabricated through spark plasma sintering (SPS) and hot-forging. Nanosized ZrC particles with an average particle size of 56 nm were homogeneously dispersed in the FeCrAl-ZrC alloys. The addition of a small proportion of ZrC nanoparticles effectively refines the grain size and improves the strength and hardness of FeCrAl alloys. However, the ductility of FeCrAl alloys decreases gradually when the ZrC content increases from 0 wt% to 2.0 wt%. The tensile strength of SPSed FeCrAl-1.0 wt% ZrC alloy at 800 °C is 91 MPa, which is about 69% higher than that of pure FeCrAl, while the percentage elongation after fracture of FeCrAl-1.0 wt% ZrC is 15.0%, which is lower than that of FeCrAl (48.2%). To improve the ductility of FeCrAl-ZrC alloys, the SPSed samples were subjected to hot forging at 1000 °C. Through hot-forging, significant enhancement in ductility of FeCrAl-ZrC alloys was achieved without reducing the strength. The mechanical properties and microstructure of FeCrAl-1.0 wt% ZrC are stable after annealing at 1000 °C for 5 h, exhibiting superior thermal stability as compared with FeCrAl.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Jingmin Wang,Xiaolong Hu,Haizhen Ding,Xin Huang,Mingsheng Xu,Zhenzhen Li,Dong Wang,Xu Yan,Yang Lu,Yunjun Xu,Yan Chen,Paulo Cesar Morais,Yupeng Tian,Ren-Quan Zhang,Hong Bi
Commercial gadolinium-based materials have been widely used as contrast agents for magnetic resonance imaging (MRI), but the high toxicity of leaking free Gd3+ ions still raises biosafety concerns. Here, we develop a novel, safe, and efficient MRI contrast agent based on a stable Fe(III) complex of fluorine and nitrogen co-doped carbon dots (F,N-CDs) that was prepared from glucose and levofloxacin by a simple microwave-assisted thermal decomposition method. The obtained Fe3+@F,N-CD complex exhibits higher longitudinal relaxivity (r1 = 5.79 mM–1·s–1) than that of the control samples of the Fe3+@CD complex (r1 = 4.23 mM–1 s–1) and free Fe3+ (r1 = 1.59 mM–1 s–1) in aqueous solution, as assessed by a 1.5 T NMR analyzer. More importantly, the Fe3+@F,N-CD complex is very stable with a large coordination constant of 1.06 × 107 in aqueous medium. While incubated with HeLa cells, the Fe3+@F,N-CD complex shows clear MR images, demonstrating that it has potential to be an excellent MRI contrast agent. Furthermore, in vivo MRI experiments indicate that the Fe3+@F,N-CD complex provides high-resolution MRI pictures of 4T1 tumor bearing BALB/c mice 15 min after injection and can be completely excreted 2 h after administration. No cytotoxicity was observed with F,N-CDs and Fe concentration up to 0.2 mg/mL and 0.3 mM in 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide cell proliferation assay, respectively. The possible mechanism of the enhanced MRI effect of the Fe3+@F,N-CD complex is therefore proposed. The extremely low toxicity, high r1 relaxivity, strong photoluminescence, and low synthetic cost enable the Fe3+@F,N-CD complex to be a safe and promising T1-weighted MRI contrast agent for clinical applications.
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ENERGY & FUELS
·
2019
·
IF 3.021
Lingjun Ma,Caixia Yue,Liang Ye,Qihuang Huo,Lina Han,Liping Chang,Weiren Bao,Jiancheng Wang
Pd–Fe bimetallic sorbents were shown to be a great potential sorbent for Hg0 removal from coal-derived fuel gas. In this work, activated carbon (AC), Al2O3, and Beta molecular sieve were chosen as supports to disperse Pd–Fe bimetallic components. The effects of the supports on Hg0 removal of Pd–Fe bimetallic sorbents were evaluated using a fixed-bed reactor at 200 °C. The regeneration performance of sorbents was also investigated. The results showed that Hg0 removal activity and regeneration performance over Pd–Fe/AC was the best, followed by Pd–Fe/Beta, and Pd–Fe/Al2O3. The Hg0 removal efficiency of Pd–Fe/AC bimetallic sorbents remained above 80% within 400 min after regeneration 4 times. The Pd–Fe bimetallic sorbents were characterized by N2 adsorption–desorption, Fourier transform infrared spectroscopy, X-ray diffraction, CO pulse adsorption, Hg temperature-programmed thermal desorption, and X-ray photoelectron spectroscopy. The analysis results revealed that three sorbents had a similar Hg0 removal mechanism. Hg0 transformed to Pd–Hg amalgam and HgS after reacting with the sorbents. Pd0 and Fe2O3 were the active species for the removal of Hg0. The removal performance of Hg0 by Pd–Fe/Al2O3 sorbents was the lowest. It is because Pd–Fe/Al2O3 sorbents have the lowest specific surface area, surface content, and dispersion degree of the Pd component. Furthermore, Pd0 over Pd–Fe/Al2O3 sorbents was severely poisoned and transformed to PdS during the regeneration process.
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CHEMOSPHERE
·
2019
·
IF 5.108
Weirui Chen,Yixiang Bao,Xukai Li,Jun Huang,Yiming Tang,Laisheng Li
Mesoporous Fe-Cu@SiO 2 core-shell catalyst was synthesized and assessed for its catalytic activity in the ozonation of salicylic acid (SA). The synthesized catalyst was characterized by XRD, TEM, SEM, XPS, H 2 -TPR, etc. Fe-Cu@SiO 2 exhibited a regular spherical shape and had the surface area at 1216 m 2 g −1 . The wrapping of metal components and their strong interaction prevented metal leaching. Fe-Cu@SiO 2 showed the highest activity for SA mineralization when compared with Fe@SiO 2 and Cu@SiO 2 . In Fe-Cu@SiO 2 /O 3 , 88% TOC was removed, which was 2.5 times as much as that in sole ozonation. SA degradation efficiency in Fe-Cu@SiO 2 /O 3 increased with initial pH. O 3 , ·OH and H 2 O 2 were the main reactive oxygen species accounting for SA mineralization. Due to their scavenging effect of ·OH, NH 4 + , NO 3 − and humic acids would inhibit the degradation efficiency of Fe-Cu@SiO 2 /O 3 . Acidic sites, oxygen vacancies and the Fe-Cu(I/II) electron transfer were responsible for ozone decomposition and ·OH generation. SA mineralization proceeded through the ·OH mechanism. Moreover, SA mineralization in O 3 and Fe-Cu@SiO 2 /O 3 both exhibited a two-stage pseudo first-order kinetics (stage I: 0–45 min; stage II: 45–120 min). The degradation intermediates were detected to investigate the reaction pathway. ORP and EEM were used to monitor the degradation process. Great difference was found for carboxylic acids accumulation in O 3 and Fe-Cu@SiO 2 /O 3 . The accelerated removal of oxalic acid and humic acid-like intermediates were responsible for the two-stage pseudo first-order kinetics.
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高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Xin Liu,Baoling Yuan,Jing Zou,Lingbin Wu,Lin Dai,Hongfang Ma,Kai Li,Jun Ma
The activation of persulfate by Fe(II) coupled with hydroxylamine (the HA/Fe(II)/PS system) was highly effective for the degradation of refractory organic contaminants under acidic pH conditions. However, owing to the precipitation of ferric hydroxide and/or the slow reduction from Fe(III) to Fe(II), the HA/Fe(II)/PS system was invalid under neutral and alkaline pH conditions. In this study, it was observed that the degradation of acid orange 7 (AO7) was strongly enhanced over the wide pH range of 2–9 when trace Cu(II) (0.5–5 μM) was spiked into the HA/Fe(II)/PS system. It was evident that Cu(I) was generated via the reduction of Cu(II) by HA in the bimetallic system at both pH 3 and pH 8, and the steady concentration of Fe(II) in the bimetallic system was much higher than that in the HA/Fe(II)/PS system due to the rapid reaction between Fe(III) and Cu(I). Quenching experiments using tert-butyl alcohol, methanol and sodium bromide as the scavengers and electron spin resonance experiments confirmed that the primary reactive species responsible for AO7 degradation were sulfate radical at both pH 3 and pH 8, rather than hydroxyl radical and Cu(III). Nevertheless, sulfate radical was mainly produced by Fe(II)-activated PS at pH 3, while both Cu(I) and Fe(II) made important contributions to the generation of sulfate radical at pH 8. The bimetallic system was also highly effective in degrading other organic contaminants, such as phenol, diclofenac, reactive red 2 and orange G. This study might provide a promising idea based on Fe(II)-activated PS for degrading organic contaminants over a wide pH range.
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