ADVANCED FUNCTIONAL MATERIALS
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2023
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IF 19
Siyu Gui,Weiwei Tang,Zhihao Huang,Xinchen Wang,Siyin Gui,Xiang Gao,Duncheng Xiao,Liming Tao,Zhengxuan Jiang,Xianwen Wang
Diabetic retinopathy (DR) is the most prevalent type of retinal vasculopathy and the most widespread cause of preventable blindness in adults. Excessive increases in reactive oxygen species (ROS) and vascular endothelial growth factor are major initiators and drivers of DR progression, respectively. However, current DR treatment options remain limited, particularly for early DR. Nanotechnology-mediated antioxidant strategies are gaining increasing popularity to treat ocular diseases. Quercetin has excellent ROS scavenging efficiency but poor stability and low bioavailability in physiological environments. In this study, ultrasmall Fe-Quer nanozymes (NZs) formed by coupling quercetin with low-toxic iron ions are reported that can mimic the activities of three important antioxidant enzymes, superoxide dismutase, catalase, and peroxidase, thereby exhibiting excellent water dispersion and efficient ROS scavenging ability. In vitro and in vivo assays validate the effects of Fe-Quer NZs against inflammation, oxidative stress damage, microvascular leakage, and angiogenesis, particularly their vascular protective effect in early DR. Transcriptomic analysis further reveals a potential multitarget-specific therapeutic mechanism of Fe-Quer NZs against DR. These observations open avenues for Fe-Quer NZs, composed of molecules of a natural product and metal ions with artificial NZ activity, as microvascular protective agents for DR and other ROS-related diseases.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Hesheng Yu,Dawei Liu,Katam Srinivas,Fei Ma,Ziheng Zhang,Mengya Wang,Yu Wu,Yue Wang,Xinsheng Li,Yuanfu Chen
It is still challenging but crucial to plumb non-noble metal-based oxygen reduction reaction (ORR) catalysts with comparable or better performance than benchmark Pt/C catalysts. Herein, we proffer an unconventional core-shell-structured iron-based heterostructure electrocatalyst constructed by a Fe/Fe 3 C heterostructure nanoparticle core wrapped by a graphitic shell embedded on a conductive N-doped mesoporous graphite skeleton (Fe/Fe 3 C@NC) via facile pyrolysis of MIL-53(Fe) (MIL = Matérial Institute Lavoisier) and melamine. The Fe/Fe 3 C@NC catalyst delivers more positive half-wave potential ( E 1/2 ) of 0.86 V and a low Tafel slope of 56 mV dec −1 for ORR, outpacing the benchmark Pt/C catalyst, and it also shows remarkable long-term durability and excellent methanol tolerance. The marvelous ORR behaviors can be attributed to its distinctive morphologic structure: the heterostructure can enhance intrinsic ORR activity; the core-shell nanostructure can enhance ORR activities through unique electron transfer between iron species and their conductive carbon shells, which can also act as protective barriers to ensure long-term stability; the high-content pyridinic-N doping can be used as additional active centers; and the abundant mesopores facilitate the diffusion of electrolyte, which can further upgrade ORR activities. This study proffers a strategy to design and fabricate non-noble catalysts with well-designed nanoarchitecture and high catalytic activity.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xuejuan Ma,Qi Ou,Jiajia Yuan,Jiaojiao Yang,Shuxia Xu,Xinfeng Zhang
Organophosphorus pesticides (OPs) are the most widely used pesticides, hence it is crucial to effectively prevent and control OPs residues for agricultural product safety and ecological development. In this work, the nanoreactor consisting of Fe-doped carbon dots (Fe-CDs) and metal-organic framework (MOF-808) were developed for selective degradation as well as sensitive detection of paraoxon and parathion. MOF-808 was selected as the host and used to rapidly degrade paraoxon due to its excellent organophosphorus hydrolase activity. Fe-CDs were severed as guest molecules not only for photocatalytic degradation of parathion, but also for sensing to detect OPs. Through host–guest interaction, Fe-CDs/MOF-808 and Fe-CDs@MOF-808 were synthesized for cascade degradation and detection of paraoxon and parathion, respectively. Paraoxon and parathion were detoxified by catalytic hydrolysis and photocatalytic degradation by Fe-CDs/MOF-808 and Fe-CDs@MOF-808, respectively. Meanwhile, the fluorescence of the nanocomposites was quenched by the internal filtering effect with 4-nitrophenol (4-NP), the degradation product of OPs. Fe-CDs/MOF-808 has a wide linear range for detection of paraoxon from 0.001 to 360 μM, with a limit of detection (LOD) as low as 0.3 nM. Fe-CDs@MOF-808 exhibited a linear range of 0.01–100 μM for parathion, with an LOD about 3.3 nM. The reliability of the nanoreactor was verified by testing the recovery rate of OPs spiked water sample. Meanwhile, the nanoreactors were applied for degradation and detection of OPs in pakchoi. The OPs in pakchoi can be fully degraded within 5 min, and the analytical results are consistent with those by standard method (HPLC). Therefore, the proposed nanoreactor provides a feasible alternative for effective degradation and timely detection of OPs during agricultural production.
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Materials Today Communications
·
2023
·
IF 3.8
Yushu Han,Rui Bao,Jianhong Yi,Hongdong Li,Liang Liu,Shuyu Huang,Zhaojie Li,Wenfu Zhang,Deqi Min
Carbonized polymer dots (CPDs) have drawn a lot of attention in the past ten years because of their excellent selectivity and sensitivity. In this study, tungsten was doped into CPDs (W-CPDs) using a simple hydrothermal technique for the first time. With an excitation/emission maximum of 365/455 nm and excitation-independent emission, W-CPDs exhibit blue fluorescence and have an average particle diameter of 2.33 nm. Because of the dynamic quenching between Fe (III) and W-CPDs, there is a good linear relationship between the Fe (III) concentration and the limit of detection (LOD) of 0.012 μM for W-CPD fluorescence intensity. The intensity of the W-CPDs fluorescence is also found to be linearly correlated with pH values between 5.0 and 10.0. This technique enables quick detection of Fe (III) in drinking water and is expected to lower the risk of Fe (III) ingestion by humans. In addition, the creation of fluorescent flexible devices and information encryption are fascinating applications for W-CPDs.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2019
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IF 4.175
Hongli Liu,Chunxiao Lv,Shuai Chen,Xiaoyang Song,Bohan Liu,Jin Sun,Huawei Zhang,Dongjiang Yang,Xilin She,Xiaoliang Zhao
The development of anode materials with a high capacity, excellent rate capability, and acceptable stability for sodium-ion batteries (SIBs) is still an urgent issue. Here, we fabricated FeS nanoparticle (NP)/three-dimensional (3D) carbon nanofiber aerogels (CNA) composites utilizing Fe-alginate aerogels as the renewable precursor. In the FeS/CNA sample, well-distributed FeS NPs were embedded on a 3D-CNA network with high electron conductivity and a large specific surface area. Impressively, the FeS/CNA sample was evaluated as an anode electrode material for SIBs, and exhibited an excellent specific capacity (473 mA h g −1 at 0.1 A g −1 ) and outstanding rate capacity (291 mA h g −1 at 5 A g −1 ). In addition, 97.4% of the capacity, 385 mA h g −1 , was retained over 400 cycles at 2 A g −1 , indicating the prominent cycling stability of the FeS/CNA sample. The results were ascribed to the unique structure of the FeS particles embedded on interconnected CNAs, which could boost sodium ion diffusion and facilitate electrolyte access.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Ranran Yuan,Cailiang Yue,Jinli Qiu,Fuqiang Liu,Aimin Li
TiO 2 @NH 2 -MIL-88B(Fe) heterostructures (TMFe-x) were successfully synthesized and used in an efficient sunlight-driven reduction towards Cr(VI) in a neutral aqueous media. Further, the prepared TMFe-x heterostructures exhibited higher photocatalytic activity when compared with those exhibited by pure TiO 2 and NH 2 -MIL-88B(Fe) under simulated sunlight irradiation. The optical TiO 2 modification content was determined to be 10 wt.% (TMFe-b), with 98.6% Cr(VI) being converted to Cr(III) within 35 min using ammonium oxalate as the hole scavenger at pH = 7. In neutral conditions, the kinetic rate constant (0.0878 min −1 ) was five times larger than the published values. Additionally, the photocatalytic performance of TMFe-b was maintained and Fe leaching was observed to be negligible after the completion of four reaction cycles. The superior photocatalytic property can be attributed to the high photoelectron-hole separation and migration efficiency. Subsequently, TMFe-b achieved Cr(VI) reduction under neutral conditions by capturing hydrogen from the water molecules or the hole scavengers. The photoelectrons and superoxide radicals were the main active species. Furthermore, TMFe-b was able to efficiently eliminate various pollutants through photocatalytic oxidation and reduction. This study suggests a novel strategy for the preparation of environmentally stable and efficient MOF-based photocatalysts to efficiently eliminate various pollutants. Further, there is a huge potential for the practical application of this technology to water purification .
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CHEMOSPHERE
·
2019
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IF 5.108
Yating Jia,Fan Hu,Yuancai Lv,Yuancai Chen,Yongyou Hu
Polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants and challenges for water treatment due to their persistence and toxicity. In this study, the reduction of 2′2′4′4′-tetrabromodiphenyl ether (BDE-47) was investigated in a nano-bio-integrated system. Results showed that the introducing of P. putida could markedly accelerate the demineralization of BDE-47 in nZVI/Pd- P.p system; the continuous generation of acidic metaboliates by P. putida could decrease pH, which could alleviate the surface passivation to some extent, resulting in the releasing of Fe 2+ and high generation of H 2 O 2 , the shift in reactive oxygen species from Fe(IV) to •OH. The BDE-47 was firstly debrominated to the DE by the highly reductive [Pd·2H] generated by nZVI/Pd, then oxidized to bromophenol and phenol, catechol as well as hydroquinone via the P. putida strain and the Fenton-like system. The toxicity assays confirmed the combined system could avert generation of nocuous intermediates, and could be an alternative strategy for complete remediation of recalcitrant POPs.
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Nanomaterials
·
2019
·Vol. 9
·期 3
·402
·
IF 4.034
Hongyu Wang,Chaohai Wang,Junwen Qi,Yubo Yan,Ming Zhang,Xin Yan,Xiuyun Sun,Lianjun Wang,Jiansheng Li
Prussian blue and its analogues (PBA) based nanomaterials have been widely applied to removing pollutants in the recent years. However, easy aggregation and poor recycling largely limit their practical applications. In this work, spiderweb-like Fe-Co Prussian blue analogue/polyacrylonitrile (FCPBA/PAN) nanofibers were prepared by electrospinning and applied to degrading bisphenol-A (BPA) by activating peroxymonosulfate (PMS). Detailed characterization demonstrated that a high loading of FCPBA (86% of FCPBA in FCPBA/PAN) was successfully fixed on the PAN nanofibers. 67% of BPA was removed within 240 min when 500 mg·L−1PMS and 233 mg·L−1FCPBA/PAN were introduced in 20 mg·L−1BPA solution at initial pH of 2.8. Electron paramagnetic resonance (EPR) and radical inhibition experiments were performed to identify the possible degradation mechanism. For comparison, a low loading of FCPBA nanofibers (0.6FCPBA/PAN nanofibers, 43% of FCPBA in FCPBA/PAN) were also prepared and tested the catalytic performance. The results showed that the activity of FCPBA/PAN was much higher than 0.6FCPBA/PAN. Furthermore, a FCPBA/PAN packed column was made as a reactor to demonstrate the reusability and stability of FCPBA/PAN nanofibers, which also exhibited the bright future for the industrial application. This work makes it possible to fabricate efficient PBA nanocatalysts with excellent recyclability and promotes the application of PBA in industrial areas.Keywords:Fe-Co Prussian blue analogues;electrospinning;peroxymonosulfate;BPA
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2018
·Vol. 219
·期 24
·1800403
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IF 2.492
Chunyan Zhang,Jianxin Luo,Wenjun Li,Lijuan Ou,Guipeng Yu,Chunyue Pan
An environment-friendly synthesis of a covalently bonded terbium(Tb)-complex-containing monodispersed fluorescent porous copolymer microspheres, and their highly selective detection of Fe 3+ are described. The as-made copolymer microspheres exhibit intense green fluorescence originating from Tb ions and high photostability in water. Encouragingly, the fluorescence of the copolymer microspheres can be selectively quenched by trace Fe 3+ due to the interaction between Fe 3+ and the ligands, which disturbs the coordination structure of Tb-complexes and inhibits the energy transfer from ligands to Tb ions. The intense fluorescence intensity, high fluorescence stability, together with the nanoscale and porous nature of the copolymer microsphere endows them with wide detection range (0–1500 µ m ) and low detection limit (2.1 µ m ) for selective recognition of Fe 3+ in aqueous environment. This study paves a new pathway for the function of porous copolymer microspheres being used as targeting for biological detection and environmental issues.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
·
IF 2.931
Zheng Fu,Jiantong He,Fengchun Jia,Mengjiao Wang,Fengling Cui
Since thiosemicarbazide contains numerous nitrogen and sulfur atoms in its structural formula that enhance its strong coordinating abilities with metal ions , it is always selected as the mother molecule for the design of metal-ion sensors. In this report, a thiosemicarbazide derivative (4-naphthalenyl-3-thiosemicarbazide (NTSC)) was synthesized via a single step process and covalently conjugated onto the surfaces of carbon dots (CDs). The modified CDs demonstrated excellent monodispersity, good photostability, and tunable luminescence properties. More importantly, the CDs retained a highly specific Fe 3+ recognition capacity in contrast to other competing metal ions . Fe 3+ can efficiently quench the fluorescence of CDs even at fairly low concentration (30 μM) with a detection limit as low as 1.68 nM. The fluorescence quenching kinetics are likely to involve static quenching, which is caused by specific interactions between NTSC-CDs and Fe 3+ toward the formation of a ground state complex. Due to their excellent optical performance, low toxicity, and good biocompatibility the NTSC-CDs may be applied to the imaging and monitoring of Fe 3+ in bacillus subtilis. In effect we successfully fabricated an effective fluorescent nanosensor for both the quantitative detection of Fe 3+ in aqueous solutions, and its real-time imaging in vivo.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiu-Xiu Fang,Wen-Min Liao,Jian-Dong Song,Wen-Zhi Jia,Yun Wang,Ji-Qing Lu,Meng-Fei Luo
A series of 3V-xFe/MgF 2 catalysts with different V/Fe molar ratios were prepared by a sol-gel method, and the effect of Fe promotion on the catalytic performance of gas-phase dehydrofluorination of 1,1,1,3,3-pentafluoropropane (HFC-245fa) was investigated. It was found that proper V/Fe ratio was helpful to improve the activity. The 3V-0.5Fe/MgF 2 catalyst (with a V/Fe ratio of 6/1) gave a HFC-245fa conversion of 76.6% at 320 °C, which was 13.4% higher than that on the 3V/MgF 2 (63.2%). The synergy between V and Fe species resulted in enhanced surface acidity which accounts for the enhanced activity. The VO x and FeO x species in the fresh catalyst could be transformed to VOF x and FeF 3 species during the reaction, which were regarded as the active sites. However, higher content of Fe in the catalyst resulted in the partial coverage of V species, which led to decline of surface acidity and thus the suppressed activity. Also, surface carbon deposition was responsible for the slight catalyst deactivation .
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Xiao-Cheng Liu,Wen-Qiang Li,Yi-Ran Wang,Guan-Nan Zhou,Yi-Xuan Wang,Chuan-Shu He,Gong-Ming Wang,Yang Mu
Promotion of iron solubility using ligands is the preliminary step in the homogeneous electro-Fenton (EF) process at a mild pH, but the chelate efficiencies of most organic ligands are unsatisfactory, resulting in insufficient Fe(II) availability. In this study, atomic H* was, for the first time, introduced to the EF process to accelerate the regeneration of the Fe(II)-complex at a mild pH using a Ni-deposited carbon felt (Ni-CF) cathode. The introduction of atomic H* significantly elevated total organic carbon (TOC) abatement of ciprofloxacin (CIP) from 42% (CF) to 81% (Ni-CF) at a natural pH. In the presence of humic acids (HAs), atomic H* introduced via Ni-CF enhanced the CIP degradation rate to 10 times that of the CF at a mild pH. The electron spin resonance (ESR), density functional theory (DFT) calculations, electrochemical characterization, and in situ electrochemical Raman study clearly demonstrated that the atomic H* generated from the Ni-CF cathode was highly efficient at reducing Fe(III)-complexes at a natural pH. Additionally, the Ni-CF could generate atomic H* without significant nickel leaching. Thus, the atomic H* could continuously facilitate iron cycling and, consequently, enhance pollutant mineralization via the homogeneous EF process at a mild pH in an environmentally friendly manner.
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