APPLIED CLAY SCIENCE
·
2012
·
IF 2.474
Zhujian Huang,Pingxiao Wu,Xing Zhang,Xiaorong Wang,Nengwu Zhu,Jinhua Wu,Ping Li
In this study, intercalation of Fe(III) complexes [Fe(Ox) 3 ] 3− and [Fe(Cit) 2 ] 3− in Mg 2 Al layered double hydroxides (LDHs) had been carried out by different routes: direct self-assembly, reconstruction and anion exchange. The result of XRD indicated that these two kinds of Fe(III) complexes intercalated LDHs (LDHs/Fe-complexes) could be successfully synthesized by anion exchange obtaining two well crystallized LDHs both with a large basal spacing. The chemical environment of iron ion in the intercalated Fe complexes was determined by FTIR , XPS and XAFS, the results of which concertedly proved that the intercalated Fe complexes were well preserved in the interlayer of LDHs. The arrangement of the Fe(III) complexes anions in the galleries of LDHs was studied by one-dimensional electron density projection. The results showed that the [Fe(Ox) 3 ] 3− anions were probably accommodated in the gallery of LDHs as an interdigitated bilayer arrangement, and the [Fe(Cit) 2 ] 3− were perpendicularly arranged against the LDHs sheets. Through the research, it is proved that the obtained LDHs/Fe-complexes markedly enhanced the UV–vis absorption ability of Fe complexes.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 42
·19811-19824
·
IF 3.5
Liu Weinan,Zhang Haiyang,Yuan Hang,Wang Lidong,Li Zhen
Peroxymonosulfate (PMS) is widely used in advanced oxidation processes. Fe(II) is an excellent catalyst for PMS, and organic pollutants in water can be effectively degraded in the Fe(II)/PMS system. However, the pollutant degradation efficiency is limited by the low conversion efficiency of Fe(II). Natural antioxidants exist in the water environment and have strong electron-donating ability. At present, the research on the introduction of natural antioxidants into the advanced oxidation processes to degrade pollutants focuses on a few polyphenols, and the effects of other natural antioxidants on the removal of pollutants are worth studying. In this study, natural antioxidants, proanthocyanidins (PCs), saponins (SPs), and Lycium barbarum polysaccharides (LBPs), were introduced into the Fe(III)/PMS system. The reduction ability of natural antioxidants was used to improve the conversion efficiency of Fe(III) to Fe(II), and PMS was more effectively activated to produce ROS, which promoted the degradation of ofloxacin (OFL). After the introduction of PC in the Fe(III)/PMS system, 80% of OFL was degraded at 20 min, and 90% of OFL was degraded at 120 min after the introduction of SP. The experimental results showed that the degradation of OFL was affected by the amount of antioxidants, PMS and Fe(III), pH value, and coexisting anions. Free radical quenching experiments showed that 1 O 2 , SO 4 − ·, and ·OH play an important role in the degradation of OFL in the Fe(III)/antioxidant/PMS system. This paper proves that the introduction of proanthocyanidins and saponins into the advanced oxidation processes can remove organic pollutants more efficiently. Graphical
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ENVIRONMENTAL TECHNOLOGY
·
2024
·
IF 2.2
Yiqing Liu,Linghan Xu,Xin Li,Shixiang Wang
Ascorbic acid (AA) was used as a reducing agent to improve the Fe(III)-activated peracetic acid (PAA) system for the removal of sulfamethoxazole (SMX) in this work. The efficiency, influencing factors and mechanism of SMX elimination in the AA/Fe(III)/PAA process were studied. The results exhibited that AA facilitated the reduction of Fe(III) to Fe(II) and subsequently improved the activation of PAA and H2O2. Various radicals, including organic radicals (e.g. CH3C(O)O• and CH3C(O)OO•) and hydroxyl radical (HO•), were rapidly formed from the activated PAA and H2O2, resulting in SMX removal. Increasing dosages of PAA and Fe(III) contributed to enhanced SMX degradation, while excessive PAA and Fe(III) did not further promote SMX degradation. Due to the radicals' quenching effect, excess AA hindered SMX elimination in the AA/Fe(III)/PAA process. The presence of HCO3− and Cl− inhibited SMX removal in this system, whereas NO3−, SO42− and natural organic matter had little impact on SMX degradation. The transformation pathways of SMX in the AA/Fe(III)/PAA system included hydroxylation, bond cleavage and amino oxidation. This research provides a strategy to enhance the Fe(III)-activated PAA system for the elimination of refractory organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Huihui Liu,Jie Zhao,Yu Wang,Yanlin Wu,Wenbo Dong,Minghua Nie,Xiaoning Wang
Peroxymonosulfate (PMS) is more cost-effective than peroxydisulfate (PDS) and has drawn great attention presently. Low efficiency of Fe(III)/Fe(II) cycle is a great intrinsic drawback of Fenton-like system, which extremely limits its widespread application. In this study, sinapic acid (SA) as a natural and environmental-friendly reductant, was applied to enhance Fe(III)/Fe(II) cycle in PMS/Fe(III) system. The removal efficiency of methyl paraben (MEP) was 98.3% (7.2 × 10 −4 s −1 ) within 90 min in the modified system, and the k obs was 18 times higher than in PMS/Fe(II) system. For the active species identification, SO 4 − , HO and Fe(Ⅳ) were all responsible for MEP degradation, while SO 4 − was the dominant radical. The role of SA in SA/PMS/Fe(III) system was investigated, Fe(III) was reduced to Fe(II) and SA was oxidized to quinone species in this reaction process. The concentration of Fe(II) and the activation efficiency of PMS were all improved with SA concentration increasing from 5 to 20 μM, and the contribution of active species for MEP degradation were estimated. The effect of initial pH and common anions were also investigated. For the effect of anions, HCO 3 − and SO 4 2− presented inhibition effect on MEP removal, and with the HCO 3 − concentration increasing 1–10 mM the inhibition decreased. Low concentration Cl − promoted MEP degradation while Cl − with higher concentration exhibited inhibition. And NO 3 − was almost no effect on MEP degradation.
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2025
·Vol. 40
·期 2
·382-388
·
IF 1.1
Cao Tian,Li Wei,Ren Lin,Song Tao,Song Jie,Lin Jiacheng,Yang Li,Liu Wenxiu,Wang Ping,Feng Shaojie
The adsorption of phosphate was conducted by the complex of chitosan/polyacrylamide/ferric(CS/PAM/Fe(III)) prepared. The SEM images and XPS spectra confirmed the successful adsorption of phosphate. The adsorption process was studied by varying the influencing aspects like pH, co-existing ions, contact time, and initial phosphate concentration. The experimental results indicate that the adsorptive capacity decreases with the increase of pH. However, it is commendable that there is still a adsorption capacity of more than 5 mg/g when the pH is 8–11. The adsorption kinetics can be accurately described by the pseudo-second-order model and is controlled by both chemisorption and surface diffusion. The adsorption process is a single layer adsorption. This paper proposed that the adsorption mechanism of CS/PAM/Fe(III) complex is the joint action of electrostatic attraction and ligand exchange.
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JOURNAL OF STRUCTURAL CHEMISTRY
·
2022
·Vol. 63
·期 4
·634-641
·
IF 1.004
Wu G. L.,Zheng C. Y.
Abstract [Fe III (OMe)(Hedtb)](ClO 4 ) 3 ·6.5CH 3 OH ( 1 ) and [Fe III (O n- Bu)(Hedtb)](ClO 4 ) 3 ·3 n -BuOH ( 2 ) (edtb = N,N,N′,N′-tetrakis[(2-benzimidazolyl)methyl]-1,2-ethanediamine) were prepared and display lipoxygenase activity. X-ray crystallography reveals that the Fe III centers in complexes 1 and 2 are ligated to three nitrogens of benzimidazole and two alkylamine nitrogen atoms from the edtb ligand, with a terminal alkyoxyl group occupying the sixth position. Complexes 1 and 2 both possess a Fe III –O R center ( R = Me, 1 ; n -Bu, 2 ) with Fe–O bond distances of 1.799(3) Å and 1.789(5) Å, respectively. The UV-Vis spectra and electrochemical properties of the complexes were recorded. Both complexes have strong absorption peaks at around 375 nm and display lipoxygenase activity.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Ruobai Li,Zhiming Chen,Meixuan Cai,Jiaxing Huang,Ping Chen,Guoguang Liu,Wenying Lv
Metal-organic frameworks (MOFs) have attracted tremendous interest as photocatalysis for the destruction of organic contaminants. Herein, we synthesize a Fe-based MOF namely MIL-53(Fe), combined with Fe(III) and percarbonate, exhibits photocatalytic activity for the destruction of Sulfamethazine (SMT) under visible LED light irradiation. The morphology and physicochemical properties of the MIL-53(Fe) were determined using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectra (EDS), Fourier transform infrared spectroscopy (FTIR) and photoluminescence spectroscopy (PL). The results indicated that the photocatalytic performance of MIL-53(Fe) with unsatisfactory efficiency resulted from the rapid recombination of photogenerated electrons and holes. This may be suppressed through the introduction of an external electron acceptor (e.g., Fe(III) and percarbonate) to the catalytic process. It could be seen that the SMT degradation efficiency in the system of Vis/MIL-53(Fe)/Fe(III)/SPC attained nearly 90% within 60 min, while only 12% achieved in the system of Vis/MIL-53(Fe). The quenching experiments and EPR analysis were employed to illuminate the predominant reactive species in the system of Vis/MIL-53(Fe)/Fe(III)/SPC. It must be mentioned that the higher separation efficiency of photoinduced electron- hole pairs was achieved via the addition of Fe(III). The accelerated photocatalytic degradation of SMT could be attributed to the subsequent formation of reactive species, which were generated from the activation of SPS by Fe(II) reduced from Fe(III) in the Vis/MIL-53(Fe)/Fe(III)/SPC system. Furthermore, the mineralization of SMT was systematically investigated, as well as the effects of operating parameters (e.g., the dose of catalyst, the concentration of Fe(III), and pH). The work has expanded the possibility of MOFs as visible light responsive photocatalysts together with percarbonate for the remediation of contaminated water.
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2D Materials
·
2025
·Vol. 13
·期 1
·015008
·
IF 4.3
Chaowei Huang,Qilin Wei,Shuaigang Ge,Xiaodong Shen,Kaihuang Huang,Bingsuo Zou
Ferromagnetic polaron (FMP) coupling and antiferromagnetic polaron (AMP) coupling have been extensively studied in zero-dimensional and three-dimensional structures. However, studying their electronic structures and photophysical processes in layer structures still faces significant challenges. In this work, we synthesized minor and rich Fe ion-doped PA2CdCl4 layer structures by slow-cooling crystallization and adjusting the Fe ion concentration. In minor Fe ion-doped PA2CdCl4, the Fe–Fe ion pair easily replaces the Cd–Cd pairs in the corner-sharing octahedra layer to form a FMP and promote a red emission (618 nm) from localized exciton-magnetic polarons (LEMPs). In the rich Fe ion doping, AMPs can be easily formed when Fe ions obtain electrons from NH2 and convert into a low-spin state, coexisting with FMPs. The increasing number of AMPs promote the formation of a new Fe-aniline charge-transfer band; the co-work of AMPs and the Fe-aniline charge-transfer band result in a blue emission (466 nm). The result of the magnetic field-dependent photoluminescence (PL) measurement indicates that the population, energy and the spin direction of AMPs and FMPs can have a direct impact on the luminescence behavior of Fe ion-doped PA2CdCl4 layered structures. The density functional theory (DFT) calculation result indicates that Fe–Fe pairs under ferromagnetic (FM) coupling interact via dx2–y2 and dz2 orbitals. Fe–Fe pairs under antiferromagnetic (AFM) coupling on the dxy and dz2 orbitals. This work provides new insights into the varied magnetic polarons of layer structures and their effect on PL behavior.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Mengxiao Zhong,Weimo Li,Junjie Chen,Siyu Ren,Ruikai Qi,Ce Wang,Xiaofeng Lu
Designing high-performance and cost-effective oxygen-evolution electrocatalysts is highly required toward sustainable water electrolysis. Surface reconstruction is a promising strategy to realize the improvement of the oxygen-evolution reaction (OER) performance of transition metal-based electrocatalysts. Herein, we present a simple electrospinning-post treatment route to construct a novel Fe(III)/NiS electrocatalyst and investigate the key role of the surface reconstruction to significantly promote the OER performance. Owing to the unique tubular morphology and the formation of the highly efficient electrochemical active species of Ni(Fe)OOH during OER process, the prepared Fe(III)/NiS nanotubular catalyst exhibits a low overpotential of 264 mV at 10 mA cm −2 , superior to the benchmark RuO 2 and many other metal sulfide electrocatalysts. Furthermore, the catalyst also presents an excellent durability with no distinct activity reduction for over 70 h. This study offers a reliable surface reconstruction way to fabricate high-efficiency and outstanding durable OER electrocatalyst, enabling it promising prospect for water electrolysis with a reduced energy consumption.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yihao Li,Hongmei Tang,Xiangqin Peng,Shiyang Tao,Jie Ding,Meiqing Chen,Pingxiao Wu,Nengwu Zhu
The dynamic interactions among iron (Fe) oxides and organic matter (OM) play vital roles in controlling the geochemical cycling of carbon (C) and toxic trace metals. Although the effects of OM on the Fe oxides transformation, and dynamic with toxic trace metals have been studied previously, it is still poor to understand the mechanistic and quantitative on the C sequestration during the Fe(III) mineralization process, and kinetics with hydrated Cu(II) in the acid drainage. In this study, Mössbauer spectroscopy, X-ray absorption spectroscopy (XAS), high resolution transmission electron microscopy (HRTEM), and density functional theory (DFT) were used to elucidate the underlying mechanism for the fine structure of iron minerals, fulvic acid (FA) sequestration and hydrated Cu(II) coordination on Fe oxides. FA dosages played an essential role in the formation of Fe oxides, which can inhibit the formation of Fe-O octahedrons and benefit to the Fe-O tetrahedron. FA molecules were mainly sequestrated on the surfaces of Fe oxides and van der Waals forces were the main interaction between FA and Fe oxides. The hydrated Cu(II) oxides mainly distributed on the surface of iron oxides as divalent oxidation states, and feasible coordinated with phenolic hydroxyl group of FA and Fe oxides. The knowledge of the dynamic coupling between Fe oxide transformation under the effect of FA and the fate of hydrated Cu(II) on Fe oxides provided the basis for predicting the geochemical process of Fe, C and toxic trace metals.
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Advanced Healthcare Materials
·
2021
·Vol. 11
·期 2
·2101926
·
IF 9.933
Wenjie Feng,Wanrui Shi,Shuwei Liu,Huiwen Liu,Yi Liu,Pengfei Ge,Hao Zhang
Most of the antitumor chemotherapeutic drugs execute the therapeutic performance upon eliciting tumor cell apoptosis, which may cause chemoresistance of tumors. Design of novel drugs to eradicate apoptosis-resistant tumors via non-apoptotic cell death pathways is promising for improving the long-term chemotherapeutic efficacy. Herein, a Fe(III)-Shikonin metal-polyphenol-coordinated supramolecular nanomedicine for combined therapy of tumor via ferroptosis and necroptosis is designed. The construction of the nanomedicine based on the coordinated self-assembly between Fe 3+ and Shikonin not only overcomes the shortcomings of Shikonin including its low bioavailability and high toxicity toward normal tissues, but also integrates the theranostics functions of Fe ions. Under the exposure of the high concentration of glutathione (GSH) in tumor cells, the as-prepared nanomedicine will disassemble into Fe 2+ and Shikonin, followed by stimulating the tumor cell death through ferroptosis and necroptosis. In addition, benefiting from the stealth effect of polyethylene glycol (PEG) and the targeting ability of cyclo(Arg-Gly-Asp- d -Phe-Lys) (cRGD) to α v β 3 -integrin, NH 2 -PEG-cRGD-modified nanomedicine exhibits a GSH-responsive therapy toward 4T1 tumor in vivo and self-enhanced longitudinal relaxation (T 1 )-weighted imaging property. Since the self-assembly of natural Shikonin and human body-necessary Fe element is facile and feasible, the work may provide a promising supramolecular nanomedicine for next-generation chemotherapeutic applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2020
·
IF 7.864
Di Huang,Jinzhao Wang,Hongling Xia,Yue Zhang,Fengxia Bao,Meng Li,Chuncheng Chen,Jincai Zhao
Both Fe(III) and fatty acids are ubiquitous and important species in environmental waters. Because they are amphipathic, many fatty acids are surface active and prone to enrichment at the air–water interface. Here, we report that by using nonanoic acid (NA) as a model fatty acid, coexisting Fe(III), even at concentrations as low as 1 μM, markedly enhanced the photochemical release of NA-derived volatile organic compounds (VOCs) such as octanal and octane into the air. Further studies indicated that the surface-enriched fatty acids dramatically increase the local concentration of Fe(III) at the water surface, which enables Fe(III)-mediated photochemical reactions to take place at the air–water interface, and the VOCs facilely produced by fatty acid photooxidation can then be released into the air. Moreover, the product distribution in the Fe(III)-mediated reactions was largely different from that in other photochemical systems, and a mechanism based on photochemical decarboxylation is proposed. Considering that the coexistence of fatty acids and Fe(III) in the environment is common, the enhanced photochemical release of VOCs by surface-enriched fatty acids and Fe(III) may be an important channel for the atmospheric emission of VOCs, which are known to play an essential role in the formation of ozone and secondary organic aerosols.
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