ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Xiang Liang,Wenhui Feng,Dong Liang,Yan Xu,Xiaoqing Qiu
Hydroxyl/amino and Fe(III) co-grafted graphite carbon nitride (CN) is fabricated via alkaline hydrothermal treatment and followed by an impregnation adsorption process. In this unique fabrication, hydroxyl and amino groups enriched on the surface play a vital role in improving the adsorption capacity for volatile organic compounds (VOCs), while the grafted amorphous Fe(III) clusters could dominantly regulate the path of molecular oxygen activation via photo-Fenton reaction, and change the selectivity of intermediate reactive oxygen species (ROS) with the assistant of the rich surficial hydroxyl groups. Meanwhile, both the grafted functional groups and Fe(III) clusters can serve as photogenerated charge acceptors for collaboratively accelerating carriers' separation. Besides, the Fe(III)-mediated interfacial charge transfer effect (IFCT) also could extend visible light absorption and boost carriers’ generation. Benefiting from the virtues of the complementary and synergy of the grafted hydroxyl/amino and Fe(III), the dual-functionalized CN is qualified as an efficient photocatalyst for removal of VOCs, which exhibits 22 and 18 times isopropanol (IPA) adsorption capacity and CO 2 production than of pristine CN during photocatalytic IPA removal, respectively. Moreover, this work provides a new strategy of surficial group-cluster bifunctionalization for systematically improving sustainable solar-to-chemical energy conversion towards VOCs mineralization.
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NANOTECHNOLOGY
·
2019
·Vol. 31
·期 1
·015101
·
IF 3.399
Keke Du,Qianqian Liu,Mei Liu,Rongmu Lv,Nongyue He,Zhifei Wang
Increasing the content of reactive oxygen species (ROS) with the assistance of nanoformulations in cancer cells via the Fenton reaction is considered an effective method to treat cancer. However, the efficiency of the Fenton reaction is affected by the level of H2O2, the selection of iron ions in different nanoformulations, etc. Herein, we use FeIII-tannic acid (FeIIITA) nanocomposites as the carrier to deliver glucose oxidase (GOD) which can solve the problem of insufficient endogenous H2O2 by catalytically converting the glucose. In comparison with traditional Fe2+/Fe3+, FeIIITA nanocomposites perform higher catalytic activity in converting H2O2 to high toxic hydroxyl radicals (·OH) due to the TA-mediated reduction of Fe3+. So, the integration of GOD and TA in the construction of nanocomposites significantly enhances the efficiency of the Fenton reaction. In vitro experiments show that ·OH produced by GOD-FeIIITA nanocomposites can not only achieve a good anticancer effect at a low concentration but also promote degradability of the nanocomposites. When it is only 1.08 μg · ml−1, the cell apoptosis rate has reached 76.91%. In vivo experiments further demonstrate that GOD-FeIIITA nanocomposites can significantly inhibit tumor growth. So this work lays a good foundation for Fenton reaction-based cancer treatment.
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HYDROMETALLURGY
·
2019
·
IF 3.465
Guang-jin Zhu,Hai-yan Tang,Hong-ling Zhang,Li-li Pei,Peng Zhou,Yi-lang Shi,Zai-hua Cai,Hong-bin Xu,Yi Zhang
An ion-imprinted polymer (IIP) was synthesized by radical copolymerization for use in the removal of trace Fe(III) ions from Cr(III)-containing solutions. During the synthesis process, Fe(III) ions, acrylic acid and ethylene glycol dimethacrylate were employed as the template ions, functional monomer and cross-linker, respectively. The optimal mole ratio of acrylic acid to Fe(III) ions, which significantly affected the adsorption performance, was determined. The maximum static adsorption capacity of the polymer for Fe(III) ions was 114.25 mg g −1 , with a selective factor ( k ) of 492.18 and a relative selective factor ( k′ ) of 50.87 for Fe(III)/Cr(III). The Fe(III) ions removal efficiency could reach 94.43%, leading to a final Fe(III) concentration of 0.053 mg L −1 in the treated solution. After the removal process, the mass ratio of Cr(III) ions to Fe(III) ions was higher than 26, 000:1 in the solution, with an initial mass ratio of Cr(III) to Fe(III) ions of 1500:1.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tao Pan,Yu Wang,Xin Yang,Xiong-fei Huang,Rong-liang Qiu
Fe(II)-catalyzed peroxymonosulfate (PMS) activation process was able to degrade persistent organic pollutants, such as polybrominated diphenyl ethers (PBDEs), but the slow transformation rate from the generated Fe(III) to Fe(II) restricted the efficiency of this process. In this study, we found that the addition of small quantities of gallic acid (GA), a model compound of natural polyphenols, in the Fe(III)/PMS process (namely GA/Fe(III)/PMS process) could exert a long-term influence on Fe(II) recycle and accelerated the degradation of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) over 72 h. Under conditions of 20.3 µM GA, 13.6 µM Fe(III) and 400 µM PMS, the degradation efficiency of BDE47 reached 85%, which was 9.4 times higher than that in the Fe(III)/PMS process. The degradation kinetics can be divided into an initial “fast stage” (k obs1 = 0.298 h −1 ) and a second “slow stage” (k obs2 = 0.021 h −1 ). Aromatic radicals such as hydroxycyclohexadienyl radical (poly-HCD ) produced by the attack of SO 4 − /HO on GA was proposed to be responsible for Fe(II) recycle in the first stage, while ring-opened products following SO 4 − /HO attack of GA-quinone mainly initiated Fe(III) reduction in the second stage. Owing to the multiple Fe(III) reduction pathways, PMS would be continuously activated by Fe(II) to form SO 4 − and HO , which were the dominant reactive species for BDE47 degradation. Finally, natural polyphenols extracted from green tea were proven effective in enhancing BDE47 degradation in Fe(III)/PMS process. This study not only provides a new way to propagate Fe(II)-activated persulfate chain reactions for the degradation of refractory organic contaminants, like PBDEs, but also sheds new insight into the reactivity of organic byproducts toward Fe in PMS-based oxidation system.
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ADVANCED FUNCTIONAL MATERIALS
·
2019
·Vol. 29
·期 36
·1904056
·
IF 15.621
Jing Zhu,Chengchao Chu,Dongsheng Li,Xin Pang,Huili Zheng,Junqing Wang,Yesi Shi,Yang Zhang,Yi Cheng,En Ren,Jingliang Cheng,Xiaoyuan Chen,Gang Liu
To address the urgent need for effective sonodynamic therapy (SDT), a facile and efficient strategy is developed for fabricating a new class of sonotheranostics. Herein, a Fe(III)-porphyrin nano-sonosensitizer is prepared by a one-step coordination synthesis, and then anchored with Bis(DPA-Zn)-RGD and manganese superoxide dismutase (SOD2) siRNA. Benefiting from the delicate interactions of the Fe(III)-coordinated nanoformulations, a highly potent sono/gene combinational therapy guided by fluorescence/magnetic resonance imaging is achieved. Importantly, this sonotheranostics significantly enhances the SDT effect of porphyrin through the cancer-targeted delivery capability and enhanced reactive oxygen species production via triple-regulated approaches, including down-regulation of SOD2, depletion of glutathione, and generation of Fenton reaction. This work opens up new perspectives for developing versatile sonotheranostics to overcome the clinical challenges of SDT.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Changjian Li,Yueqi Wang,Xiaojie Zhang,Xueling Guo,Xiaoxuan Kang,Libo Du,Yang Liu
Carbon dots have attracted considerable attention in the field of biosensors and bioimaging because of their excellent optical performance and low toxicity. However, the cellular uptake of the reported carbon dots generally has a low efficiency, which limits their practical applications. In this study, we reported a novel red fluorescent sulfur and nitrogen co-doped carbon dots with small molecular phenylboronic acid tags (i.e. S, N-CDs-PBA). The S, N-CDs-PBA can be taken up rapidly by PC12 cells in twenty minutes and showed high sensitivity for the detection of Fe 3+ ions. The maximum emission wavelength is at 593 nm under the excitation of 550 nm. The absolute fluorescence quantum yield is 23% in water. The fluorescence can be effectively and selectively quenched by Fe 3+ ions and the linear response range of Fe 3+ ions was obtained from 0.3 µM to 5.0 µM with a detection limit as low as 0.1 µM. It could be concluded that the rapid uptake of S, N-CDs-PBA into cells and high photoluminescence quantum yield of red emission are beneficial for quick detection of Fe 3+ ions.
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ENVIRONMENTAL TOXICOLOGY AND PHARMACOLOGY
·
2018
·
IF 2.776
Chen Zhou,Huiqing Wang,Youbin Si,Kang Wu,Amina Yousaf
The ability of anthraquinone-2,6-disulfonate (AQDS) and riboflavin to enhance the sulfamethoxazole (SMX) degradation coupled with the Fe(III) reduction by Shewanella oneidensis MR-1 was investigated. The results indicated that the SMX degradation rate was 38.5% with an initial SMX concentration at 0.04 mM. For the overall performance of AQDS and riboflavin mediated SMX degradation and iron reduction, the SMX degradation rate was gradually increased with the enhancement of iron reduction. Riboflavin had a stronger enhancement on SMX degradation and iron reduction than AQDS, but the enhancement was not positively correlated with electron shuttles concentration. A quantitative characterization of the electron transfer capacity (ETC) of the electron shuttles showed that the ETC was higher for riboflavin than AQDS. The S. oneidensis MR-1 16S rRNA gene copies results indicated that electron shuttles had a positive effect on the microbial activity of S. oneidensis MR-1. The LC MS result indicated that the products of the SMX biodegradation were 3-amino-5-methylisoxazole and 4-aminobenzenesulfonic acid, which suggested that the SMX biodegradation was caused by S N bond cleavage. This study indicates that the biochemical mechanisms play a vital role in SMX transformation and Fe(II) generation in this system.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 30
·15797-15807
·
IF 8.867
Dan Zhao,Xiao-Hui Liu,Yue Zhao,Peng Wang,Yi Liu,Mohammad Azam,Saud I. Al-Resayes,Yi Lu,Wei-Yin Sun
Excess and deficiency of iron(III) and antibiotics from normal permissible limits will induce serious disorders, so their detection is important but challenging. In this work, by introducing a new amino triazole ligand N1-(4-(1H-1,2,4-triazole-1-yl)benzyl)-N1-(2-aminoethyl)ethane-1,2-diamine (L), a series of Cd(II)-based metal–organic frameworks (MOFs) [Cd3(BDC)3(DMF)2] (1), [Cd(L)(BDC)]2·2DMF·H2O (2), [NaCd2(L)(BDC)2.5]·9H2O (3), [Cd2(L)(2,6-NDC)2]·DMF·5H2O (4) and [Cd2(L)(BPDC)2]·DMF·9H2O (5) were synthesized. MOFs 1, 2 and 3 obtained under the same conditions with the same auxiliary ligand (H2BDC) but different amounts of alkali (NaOH) show distinct 3D, 1D and 3D framework structures, respectively, in which L and BDC2− exhibit varied coordination modes. 4 and 5 with 3D structures were isolated by using longer auxiliary ligands of 2,6-H2NDC and H2BPDC. The porosity and excellent fluorescence performance of 3, 4 and 5 make them potential luminescent sensors for Fe(III) and antibiotics. The results show that 3, 4 and 5 represent high sensitivity for the detection of Fe(III) ions with detection limits of 155 ppb for 3, 209 ppb for 4 and 297 ppb for 5 due to the existence of open channels and chelating NH2 sites. In addition, the strong emissions of 3, 4 and 5 can be quenched efficiently by trace amounts of NFs (nitrofurazone, NZF; nitrofurantoin, NFT; furazolidone, FZD) antibiotics even in the presence of other competing antibiotics such as β-lactams (penicillin, PCL). They are responsive to NZF with detection limits of 162 ppb for 3, 75 ppb for 4 and 60 ppb for 5.
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CHEMICAL PHYSICS LETTERS
·
2017
·
IF 1.815
Shiliang Wei,Kun Jia,Hongguo Shou,Xuefei Zhou,Pan Wang,Xiaobo Liu
Polyarylene ether nitrile (PEN) is traditionally used as high performance thermoplastics in various advanced engineering materials fields. However, the preparation of optically active PEN based materials, especially in aqueous solution, is still a great challenge. In this work, the side chain carboxylated PEN can be readily dissolved in alkaline solution but showing strongly quenched luminescence. Fortunately, the cationic surfactant of cetyltrimethylammonium bromide (CTAB) was able to recover the fluorescence emission of water soluble PEN, which can be subsequently quenched by Fe 3+ ions, leading to the selective determination of Fe 3+ ions in aqueous solution.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Cheng Wang,Wenfeng Tan,Xionghan Feng
Iron-based sulfite (S(IV)) activation has emerged as a novel strategy to generate sulfate radicals (SO 4 •- ) for contaminants degradation. However, numerous studies focused on dissolved iron-induced homogeneous activation processes while the potential of structural Fe(III) remains unclear. In this study, five iron (hydr)oxide soil minerals (FeO x ) including ferrihydrite , schwertmannite , lepidocrocite , goethite and hematite , were successfully employed as sources of structural Fe(III) for S(IV) activation. Results showed that the catalytical ability of structural Fe(III) primarily depended on the crystallinity of FeO x instead of their specific surface area and particle size, with ferrihydrite and schwertmannite being the most active. Furthermore, in-situ ATR-FTIR spectroscopy and 2D-COS analysis revealed that HSO 3 - was initially adsorbed on FeO 6 octahedrons of FeO x via monodentate inner-sphere complexation, ultimately oxidized into SO 4 2- which was then re-adsorbed via outer-sphere complexation. During this process, strong oxidizing SO 4 •- and •OH were formed for pollutants degradation , confirmed by radical quenching experiments and electron spin resonance . Moreover, FeO x /S(IV) system exhibited superior applicability with respect to recycling test, real waters and twenty-six pollutants degradation. Eventually, plausible degradation pathways of three typical pollutants were proposed. This study highlights the feasibility of structural Fe(III)-containing soil minerals for S(IV) activation in wastewater treatment .
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WATER RESEARCH
·
2025
·
IF 12.4
Yang Wang,Ziyuan Huang,Zhang Yan,Zhenchao Lei,Huanxin Ma,Chunhua Feng
Acid mine drainage (AMD) is characterized by high concentrations of Fe(II) and Fe(III), which can be harnessed for the in-situ formation of schwertmannite, enabling the efficient immobilization of toxic heavy metals. However, existing biological and chemical methods for schwertmannite synthesis face significant challenges, including low Fe(II) oxidation rates and particularly limited Fe(III) precipitation efficiency in acidic environments. In this study, we develop a visible light-assisted photo-electrochemical (PEC) system that effectively overcomes these barriers. By leveraging anodically evolved O 2 and cathodically generated OH − , we achieved facile Fe(II) oxidation at pH 3.0, and an impressive Fe(III) precipitation efficiency of 82.8 %, significantly exceeding the < 30 % efficiency reported by other methods. Mössbauer spectroscopy and X-ray diffraction confirmed that the generated minerals are high-purity schwertmannite. Experimental and theoretical analyses revealed that in the presence of cathodic alkalinity, Fe(III) undergoes further hydrolysis to form [(H₂O) 3 Fe(OH) 2 (SO 4 )] − species, which are thermodynamically capable of spontaneous polymerization and mineralization. Furthermore, the photoreduction of [(H₂O) 4 Fe(SO 4 ) 2 ] − within the PEC system, followed by subsequent oxidation, plays a crucial role in facilitating Fe(III) mineralization. The PEC system also effectively transformed As(III) to As(V) and Cr(VI) to Cr(III) in AMD, promoting their immobilization in the resultant schwertmannite.
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FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Ting Lu,Yucui Hou,Weize Wu,Muge Niu,Wei Li,Shuhang Ren
Carboxylic acids are considered as an important group of chemicals. Direct conversion of cellulose to formic acid (FA) by vanadium(V(V))-contained catalyst is of significant conceptual and practical interest. A second metal (from Mg(II), Ca(II), Al(III), Cr(III), Mo(VI), Mn(II), Cu(II), or Fe(III)) incorporated into V(V)-contained catalyst system was screened to further improve the oxidation of cellulose by O 2 to yield FA. Fe(III) exhibited the best performance and effects of reaction parameters on the conversion of cellulose in NaVO 3 -FeCl 3 -H 2 SO 4 aqueous solution were investigated. Cellulose could be rapidly converted, and the yield of FA (66.8%) was higher than that obtained by the single use of FeCl 3 (48.4%) or NaVO 3 (57.6%). The conversion of cellulose in another V(V)-contained catalyst system (H 5 PV 2 Mo 10 O 40 ) was explored to verify the universal enhancement of FeCl 3 . Influences of the second metal Fe(III) on the V(V)-contained catalyst system and mechanism of cellulose oxidation in the V(V)-Fe(III)-H 2 SO 4 system were studied. Compared with single use of V(V), the employment of Fe(III) alone is not active enough in the oxidative C C bond cleavage . V(V) other than Fe(III) is the main active species for selective oxidation of substrates. The incorporation of Fe(III) and V(V) shows both synergistic and competitive relationships. Both the synergistic and competitive effects are beneficial to increase FA yield, as they promote the oxidation of V(IV) to V(V), increase oxidative ability, and inhibit the overoxidation to by-product CO 2 . The catalyst system was reused four times without decline in activity.
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