SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hongwei Luo,Chenyang Liu,Ying Cheng,Yifeng Zeng,Dongqin He,Xiangliang Pan
The biggest problem with Fe/PMS (peroxymonosulfate) system is the slow generation rate of SO 4 − due to inefficient Fe 3+ /Fe 2+ cycle and the low decomposition efficiency of PMS . Here, we report the Fe 3+ -enhanced decomposition of PMS by a two-dimensional transition metal dichalcogenide WS 2 for pollutant degradation and E. coli disinfection. Experimental results showed that the removal rates of six representative pollutants were all above 90% under various pH conditions. Over a wide range of pH values (2–9), the removal rate of carbamazepine (CBZ) in PMS/WS 2 /Fe 3+ system almost reached 100% within 10 min, and E. coli could be inactivated by 97.3% within 1 min. WS 2 in the system accelerated the Fe 3+ /Fe 2+ cycle and participated in the activation of PMS. Electron paramagnetic resonance (EPR) measurements and scavenging experiments demonstrated that the SO 4 − and HO radicals were the main active oxidative species. The degradation pathway of CBZ was revealed based on its intermediates as determined by liquid chromatograph-mass spectrometer (LC-MS). The presence of common anions such as Cl − and HCO 3 − in PMS/WS 2 /Fe 3+ system noticeably affected the CBZ degradation. The characterization results verified the structural stability and the reusability of WS 2 . These research findings suggest that the combination of Fe 3+ and WS 2 is a promising method for PMS activation to remove organic pollutants and inactivate pathogenic bacteria during the process of wastewater treatment .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Hejun Ren,Xiong Jin,Chenguang Li,Tingting Li,Yang Liu,Rui Zhou
In this study, we reported that the presence of rosemary acid (RA) could strongly enhance the Fe(III)-mediated Fenton oxidation of 2,4-DCP as the model contaminant at near neutral pH. This enhancement was verified by the strong chelating and reducing ability of RA, which could prevent ion precipitation and accelerate the Fe 3+ /Fe 2+ cycle. Radical quenching experiments and electron paramagnetic resonance confirmed the existence and roles of hydroxyl radicals in the Fe 3+ /RA/H 2 O 2 system. Lot size optimized experiments were executed to achieve efficient 2,4-DCP degradation (99.93%) under the optimum conditions of 100 μmol/L Fe 3+ , 100 μmol l/L RA and 8 mmol/L H 2 O 2 within 60 min. In addition, co-existing metal ions , inorganic anions and natural organic matters were proved that they could inhibit removal efficiency and rate at varying degrees. Total organic carbon and chloride ion measurements were employed to probe the mineralization of organic matters (including RA and 2,4-DCP). This study provides a new modified Fenton system to enhance the oxidation removal of refractory organics in water and will enrich the understanding on effective H 2 O 2 activation at neutral pH.
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PubMed
高影响因子
LUMINESCENCE
·
2020
·Vol. 35
·期 8
·1350-1359
·
IF 1.855
Liu Zhang,Yue Hou,Xiaoyan Guo,Wei Liu,Congcong Lv,Chunyang Zhang,Yan Jin,Baoxin Li
In this study, three types of Fe(III) bipyridyl or phenanthroline (Fe(III)-L 3 ) complex could directly catalyze 3,3′,5,5′-tetramethylbenzidine (TMB) to induce blue chromogenic changes without H 2 O 2 . Fe(III)-L 3 complex could induce a colour change in TMB directly after a short incubation time. Due to the high oxidase-like activity of the Fe(III)-L 3 complexes, superoxide anion radicals (O 2 •– ) were formed in solution. Intermediates radical involving oxo-iron species were then produced that oxidized TMB to its oxidation products (oxTMB), which had an absorbance maximum at 652 nm. Glutathione (GSH) could inhibit the oxidation reaction of the Fe(III)-L 3 complex–TMB system, a rapidly colorimetric method was established for the specific detection of GSH that had a detection limit of 0.1 μM. Furthermore, Fe(III)-L 3 complexes could catalyze TMB to oxTMB directly without H 2 O 2 . This fast and simple colorimetric method may open a new avenue for application in the point-of-care diagnosis field using the TMB chromogenic system.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 36
·36410-36422
·
IF 2.914
Latif Abdul,Kai Sun,Si Youbin
This study demonstrated, for the first time, Fe(III)/peroximonosulphate (PMS) could be an efficient advanced oxidation process (AOP) for wastewater treatment. Bisphenol A (BPA) was chosen as a model pollutant in the present study. Fe(III)-activated PMS system proved very effective to eliminate 92.18% of BPA (20 mg/L) for 30-min reaction time at 0.50 mM PMS, 1.5 g/L Fe(III), pH 7.0. The maximum degradation of BPA occurred at neutral pH, while it was suppressed at both strongly acidic and alkaline conditions. Organic and inorganic ions can interfere with system efficiency either positively or negatively, so their interaction was thoroughly investigated. Furthermore, the presence of organic acids also affected BPA degradation rate, especially the addition of 10 mM citric acid decreased the degradation rate from 92.18 to 66.08%. Radical scavenging experiments showed that SO 4 •– was the dominant reactive species in Fe(III)/PMS system. A total of 5 BPA intermediates were found by using LC/MS. A possible degradation pathway was proposed which underwent through bridge cleavage and hydroxylation processes. Acute toxicity of the BPA degradation products was assessed using Escherichia coli growth inhibition test . These findings proved to be promising and economical to deal with wastewater using iron mineral for the elimination of organic pollutants.
Graphical abstract
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高影响因子
Theranostics
·
2023
·
IF 12.4
Wenjie Feng,Wanrui Shi,Yanqi Cui,Jiajun Xu,Shuwei Liu,Hang Gao,Shoujun Zhu,Yi Liu,Hao Zhang
Immunoadjuvants, as an indispensable component of tumor vaccines, can observably enhance the magnitude, breadth, and durability of antitumor immunity. However, current immunoadjuvants suffer from different issues such as weak immunogenicity, inadequate cellular internalization, poor circulation time, and mono-functional bioactivity. Methods: Herein, we construct Fe 3+ -Shikonin metal-phenolic networks (FeShik) nanomedicines as immunogenic cell death (ICD) stimulants and multifunctional immunoadjuvants for tumor vaccination. The multifunctionality of FeShik nanomedicines is investigated by loading ovalbumin (OVA) as the model antigen to construct OVA@FeShik nanovaccines or 4T1 tumor cell fragment (TF) as homologous antigen to construct TF@FeShik nanovaccines. In vitro examinations including GSH responsive, •OH generation, colloid stability, cellular uptake, cytotoxicity mechanism of ferroptosis and necroptosis, ICD effect, the promotion of DC maturation and antigen cross-presentation were studied. In vivo observations including pharmacokinetics and biodistribution, antitumor effect, abscopal effect, immune memory effect, and biosafety were performed. Results: The presence of FeShik nanomedicines can significantly prolong the blood circulation time of antigens, increasing the bioavailability of antigens. Upon phagocytosis by tumor cells, FeShik nanomedicines can disassemble into Fe 2+ and Shikonin in response to tumor microenvironments, leading to ICD of tumor cells via ferroptosis and necroptosis. Consequently, ICD-released autologous tumor cell lysates and pro-inflammatory cytokines not only stimulate DC maturation and antigen cross-presentation, but also promote macrophage repolarization and cytotoxic T lymphocyte infiltration, resulting in the activation of adaptive immune responses toward solid tumors. Conclusion: In a word, our FeShik supramolecular nanomedicines integrate bioactivities of ICD stimulants and immunoadjuvants, such as eradicating tumor cells, activating antitumor immune responses, modulating immunosuppressive tumor microenvironments, and biodegradation after immunotherapy. Encouraged by the diversity of polyphenols and metal ions, our research may provide a valuable paradigm to establish a large library for tumor vaccination.
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高影响因子
RARE METALS
·
2020
·Vol. 40
·期 7
·1957-1965
·
IF 2.161
Xu Yin-Long,Mo Rui-Xue,Qi Cai-Yu,Ren Zeng,Jia Xiu-Zhi,Kan Zi-Gui,Li Cao-Long,Wang Fei
Abstract The excitation wavelength-dependent and -independent emissions are two crucial fluorescent properties of carbon dots (CDs). However, CDs reported till date exhibit only one of these properties, which limits their practical applications. Herein, dual-property carbon dots (DCDs) with both the excitation wavelength-dependent and -independent emissions were synthesized via a facile one-step solvothermal method using 4-(2-pyridylazo)-resorcinol as the carbon precursor. The multi-functional applications of the resulting DCDs were also evaluated. The as-prepared DCDs exhibited not only excellent monodispersity, high photostability, and storage stability, but also low toxicity, good biocompatibility, and cellular bioimaging capability. In addition, the DCDs exhibited excitation-dependent emission photoluminescence under low excitation wavelengths. The DCDs exhibited good Fe 3+ detection by quenching the blue emission fluorescence and showed a relatively low Fe 3+ detection limit of 0.067 μmol·L −1 based on three times signal-to-noise criteria ( R 2 = 0.99). Furthermore, the DCDs showed excitation-independent emission at low excitation wavelengths and exhibited red emission at about 598 nm to avoid damage to the body. These results demonstrate the excellent bioimaging properties of the DCDs. Owing to their dual PL properties, the as-prepared DCDs exhibited multi-functional applications: Fe 3+ detection and A549 cell bioimaging. These results will be helpful in developing novel CDs for applications in various fields. Graphic abstract
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tong Zhang,Yuan Chen,Yurong Zhang,Bin Liu,Yuanyuan Liu,Jianwei Zhao
Cr(VI) and catechol are common pollutants in wastewaters of tannery industry. Cr(VI) reduction by catechol results in accumulation of Cr(V)-complex and toxic o -benzoquinone. Cr(VI) reduction can be enhanced by accelerating the electron transfer from catechol to Cr(VI) using Fe(III). This electron transfer allows the continuous production of reactive oxygen species (ROS) in advanced oxidation processes, which further degrades catechol. However, the effects of catechol on Fe(III)-based Cr(VI) reduction and ROS production are not clear. In this study, the electron transfer pathway between catechol, Fe(III) and Cr(VI) was investigated along with the catechol degradation by ROS. Results show that the process of Cr(VI) reduction follows well a pseudo-second-order kinetic model, and the activation energy decreases by 4189 J/mol after electrons are transferred by Fe(III). Aqueous chromium (50 mg/L) was completely precipitated as Cr(OH) 3 , Fe x Cr 1-x (OH) 3 or Fe(OH) 3 -Cr(OH) 3 at Fe(III) concentration of 10 mmol/L. Residual catechol and Fe(II) in wastewater activated percarbonate, thereby producing OH for over 480 min at pH 3.0 and generating OH and CO 3 − for over 5 min at pH 10.0. Catechol was degraded by these ROS to butenedioic, oxalic, and formic acids, which were then mineralized to H 2 O and CO 2 . Catechol (2 mmo/L) was fully removed from wastewater with TOC removal of 37%, and the degradation was not affected by SO 4 2− and Cl − . This study provides new insights into the removal of pollutants from wastewaters via electron transfer mediated by Fe(III), and may aid in controlling the toxic effects of Cr(VI) and catechol-like organics in natural and engineered aquatic systems.
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Analytical Methods
·
2023
·Vol. 15
·期 19
·2334-2342
·
IF 3.1
Qian Li,Jing Yang,Wenzhan Yu,Liqiong He,Renlong Zhou,Changming Nie,Lifu Liao,Xilin Xiao
Monocrotophos (MP), an organophosphorus pesticide, poses a serious threat to human health, so a rapid and simple technique is needed to detect it. In this study, two novel optical sensors for MP detection were created using the Fe(III) Salophen complex and Eu(III) Salophen complex, respectively. One sensor is an Fe(III) Salophen complex (I-N-Sal), which can bind MP selectively and form a supramolecule, resulting in a strong resonance light scattering (RLS) signal at 300 nm. Under the optimum conditions, the detection limit was 30 nM, the linear range was 0.1–1.1 μM, the correlation coefficient R2 = 0.9919, and the recovery rate range was 97.0–103.1%. Interaction properties between the sensor I-N-Sal and MP and the RLS mechanism were investigated using density functional theory (DFT). And another sensor is based on the Eu(III) Salophen complex and 5-aminofluorescein derivatives. The Eu(III) Salophen complex was immobilized on the surface of amino-silica gel (Sigel-NH2) particles as the solid phase receptor (ESS) of MP and 5-aminofluorescein derivatives as the fluorescent (FL)-labeled receptor (N-5-AF) of MP, which can selectively bind the MP and form a sandwich-type supramolecule. Under the optimum conditions, the detection limit was 0.4 μM, the linear range was 1.3–7.0 μM, the correlation coefficient R2 = 0.9983, and the recovery rate range was 96.6–101.1%. Interaction properties between the sensor and MP were investigated by UV-vis, FT-IR, and XRD. Both sensors were successfully applied to the determination of MP content in tap water and camellia.
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高影响因子
WATER RESEARCH
·
2019
·
IF 7.913
Shuhui Sun,Shu Wang,Yuxuan Ye,Bingcai Pan
Considerable amount of phosphorous is present as organic phosphonates (usually in the form of metal complexes, e.g., Ca(II)-phosphonate) in domestic and industrial effluents , which cannot be effectively removed by traditional processes for phosphate. Herein, we employed a proprietary process, i.e., Fe(III) displacement/UV irradiation/co-precipitation (denoted Fe(III)/UV/NaOH), to enable an efficient removal of Ca(II)-phosphonate complexes from water. The combined process includes three basic steps, i.e., Fe(III) replacement with the complexed Ca(II) to form Fe(III)-phosphonate of high photo-reactivity, UV-mediated degradation of Fe(III)-phosphonate to form phosphate and other intermediates, and the final phosphorous removal via co-precipitation at pH = 6. The operational conditions for the combined process to remove a typical phosphonate Ca(II)-NTMP (nitrilotrismethylenephosphonate) are optimized, where ∼60% NTMP is transformed to phosphate with the total phosphorous reduction from 1.81 mg/L to 0.17 mg/L. Under UV irradiation, the cleavage of NTMP is identified at the C-N and C-P bonds to form the intermediate products and phosphate in sequence. Also, the combined process is employed for treatment of two authentic effluents before and after activated sludge treatment, resulting in the phosphorous drop from 4.3 mg/L to 0.23 mg/L and from 0.90 mg/L to 0.14 mg/L respectively, which is much superior to other processes including Fenton/co-precipitation. In general, the combined process exhibits great potential for efficient removal of phosphonates from contaminated waters .
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高影响因子
FOOD CHEMISTRY
·
2018
·
IF 4.946
Nan Wang,Huijuan Chai,Xuelin Dong,Qian Zhou,Lihua Zhu
Iron(III) ethylenediaminetetraacetate (Fe(III)EDTA) is widely used in iron fortification for reducing iron deficiency, and its determination is urgently needed. The present work developed a fluorescent method to straightforwardly determine Fe(III)EDTA by using photoluminescent carbon dots (C-dots) with the aid of F − ions as the masking agent of free Fe 3+ ions. In the presence of F − ions, only Fe(III)EDTA selectively quenched the photoluminescence of C-dots, and both Fe 3+ and Fe 2+ as well as other carboxylic acids have no effect on the emission of C-dots. The sensing mechanism was attributed to the ligand-tailored electron transfer process from C-dots to Fe 3+ . Under optimum conditions, this method showed a linear calibration plot over the Fe(III)EDTA range of 1.0–200 μmol L −1 and a detection limit of 0.4 μmol L −1 . The proposed method was successfully applied to determine Fe(III)EDTA in real samples with acceptable recoveries of spikes (95%−110%) and repeatability (RSD, 4.2%−9.5%).
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高影响因子
POLYHEDRON
·
2017
·
IF 1.926
Xiu-Mei Zhang,Jie Tang,Li-Na Wang,Di Yao,Qing Yu,Fu-Ping Huang,He-Dong Bian
Mimetics of superoxide dismutases (SOD), with certain ability to eliminate superoxide radicals under aerobic conditions, would be promising as drug candidates for antioxidant therapy. Many efforts have been devoted to synthesize small molecular compounds to mimic the functionality of natural SOD. In this paper, the Mn(III)/Co(III)/Fe(III) complexes have been synthesized with the Schiff base ligand (NaH 2 L), which was condensed from 2-hydroxynaphthalen-1-naphthaldehyde and 3,4-diaminobenzenesulfonic acid. The structures of complexes 1 and 3 have been determined by X-ray crystallographic method, and all the complexes have been investigated using FT-IR, MS. The binding constants between metal complexes and bovine serum albumin (BSA) have been determined by fluorescence spectroscopy. Meanwhile, we have synthesized 3 hybrid proteins through the interaction of the complexes and BSA. The SOD-like activity was tested by xanthine/xanthine oxidase method. The result shows that BSA molecule can increase the SOD activity of the transition metal complexes.
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高影响因子
RSC Advances
·
2017
·Vol. 7
·期 46
·28637-28646
·
IF 3.108
Pei Song,Lisha Zhang,Hao Long,Meng Meng,Ting Liu,Yongmei Yin,Rimo Xi
In this research, we developed a multianalyte fluorescence sensing system through a carbon dots (CDs)-based fluorescent probe that can specifically recognize Fe(III) by fluorescence quenching. The CDs prepared using black tea by a hydrothermal method show outstanding properties like low cytotoxicity, high photostability, excellent biocompatibility, and high sensitivity. It was found that the fluorescence of CDs can be quenched by micromolar concentrations of Fe(III) in both aqueous solutions as well as living cells. It is well known that glucose can be oxidized by glucose oxidase (GOx) to release H2O2, which, in turn, can oxidize Fe(II) to Fe(III). Based on this consideration, a multianalyte sensing system was established. Therefore the quantitative analysis of Fe(III), H2O2, and glucose with detection limits of 0.25 μM, 0.82 μM, and 1.71 μM, respectively, was achieved by the simple and cost-effective multianalyte CDs sensing system constructed. The sensing system showed high photostability and negligible cytotoxicity toward HeLa cells, which enables it to be applied in the visualization of Fe(III) or H2O2 in living cells. The system was further applied in the detection of Fe(III) or glucose in human serum, and satisfactory results were obtained.
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