WATER RESEARCH
·
2022
·
IF 13.4
Siqi Liu,Andrey M. Kuznetsov,Weiqing Han,Alexei N. Masliy,Gregory V. Korshin
Methylated arsenic species are ubiquitous in the environment and resistant to removal by conventional treatment technologies. This study addressed this challenge based on the examination of the removal of dimethylarsinic acid (DMA) in a system that combines zerovalent iron (ZVI) and powdered activated carbon (PAC). The removal of DMA in the ZVI/PAC system was compared to that by coagulation, adsorption, electrochemical and Fenton oxidations, and other conventional methods. While only the electrochemical oxidation using a PbO 2 /Sb-SnO 2 /Ti anode allowed removing up to 60% DMA at several hours-long treatment times, the removal of DMA in the ZVI/PAC system containing 10 g/L ZVI and 2.5 g/L PAC with an initial pH of 2.0 was 95% for a 30 min reaction time. Specific roles of PAC, ZVI and its oxidation products in DMA removal were examined based on the spectroscopic data and quantum chemical modeling for the DMA/Fe(II) and DMA/Fe(III) systems. These methods demonstrated the formation of moderately strong DMA/Fe(II) and DMA/Fe(III) complexation. These results and relevant kinetic data were interpreted to indicate that the removal of DMA is governed by the rapid generation of Fe 2+ ions released as a result of accelerated ZVI corrosion in the galvanic ZVI/PAC microcells and ensuing formation of DMA/ Fe 2+ complexes that are readily adsorbed by PAC.
研究领域:
环境科学
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化学工程
·
水处理
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jiandong Guo,Husheng Jia,Aiqin Zhang,Zhen Pei,Man Luo,Jinbo Xue,Qianqian Shen,Xuguang Liu,Bingshe Xu
Iron-based MOFs have been considered as the candidate for Fenton-like reagents owing to their open pore size and uniformly dispersed Fe active centers. However, the strong coordination of metal ions with organic ligands greatly reduces the exposed active sites of most iron-based MOFs, thus reducing Lewis acid sites and limiting the activation efficiency of H 2 O 2 . At the same time, low Fe 3+ /Fe 2+ cycle efficiency also restricts H 2 O 2 activation efficiency. Hence, in this work, a series of MIL-100 (Fe) containing mixed valence coordinatively unsaturated metal site (CUS) with different Fe 2+ /Fe 3+ ratios was synthesized by heat treatment and used for tetracycline hydrochloride (TC-HCL) degradation with the assistance of visible light. Interestingly, accelerated Fe 3+ /Fe 2+ cycle was observed with the aid of visible light. Among the prepared samples, CUS-MIL-250 prepared under vacuum at 250℃ has superior degradation performance, primarily owing to its large specific surface area and pore volume, improved visible light absorption, and the introduction of more Fe 2+ CUS. Meanwhile, compared with Fenton-like system and photocatalytic system, the CUS-MIL-250/H 2 O 2 /Vis system, with effective separation of photogenerated electrons and holes, demonstrates a synergistic effect to generate more reactive oxidation species, thereby improving the degradation efficiency. In addition, the catalyst shows good stability and recyclability.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Small
·
2024
·Vol. 20
·期 27
·2309541
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IF 13
Tingting Liu,Kaiyue Hu,Yansheng Li,Yanhong Wang,Dongmei Han,Zhihua Wang,Fubo Gu
The Z-scheme MIL-88B/BiOBr (referred to as M x B y , whereas x and y are the mass of MIL-88B(Fe) and BiOBr) heterojunction photocatalysts are successfully prepared by a facile ball milling method. By adding low concentration H 2 O 2 under visible light irradiation, the Z-scheme heterojunction and photocatalytic-Fenton-like reaction synergistically enhance the degradation and mineralization of ciprofloxacin (CIP). Among them, M50B150 showed efficient photodegradation efficiency and excellent cycling stability, with 94.6% removal of CIP (10 mg L −1 ) by M50B150 (0.2 g L −1 ) under 90 min of visible light. In the M x B y heterojunctions, the rapid transfer of photo-generated electrons not only directly decomposed H 2 O 2 to generate · OH, but also improved the cycle of Fe 3+ /Fe 2+ pairs, which facilitated the reaction with H 2 O 2 to generate · OH and · O 2 − radicals. In addition, the effects of photocatalyst dosages, pH of CIP solution, and coexisting substances on CIP removal are systematically investigated. It is found that the photocatalytic- Fenton-like reaction can be carried out at a pH close to neutral conditions. Finally, the charge transfer mechanism of the Z-scheme is verified by electron spin resonance (ESR) signals. The ecotoxicity of CIP degradation products is estimated by the T.E.S.T tool, indicating that the constructed photocatalysis-Fenton-like system is a green wastewater treatment technology.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Wen Song,Xinyu Xiao,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
Supporting Fe catalysts on N doped carbon (Fe-N-C) renders a promising way towards peroxymonosulfate (PMS) activation for water decontamination , but constructing high-efficiency Fe-N-C remains challenging due to the insufficient understanding of the structure-performance relationship. Herein, the N doped carbon nanotube supported Fe catalysts (Fe-NCNT) were prepared towards PMS activation for organic pollutants removal, in which the Fe-N coordination number and Fe species were tuned through changing the pyrolysis temperature to study their roles in PMS activation. Results showed increasing the pyrolysis temperature converted the Fe-N 4 structure in Fe-NCNT to low-coordinated Fe-N 3 structure and produced Fe nanoparticles (FeNP, encapsulated in carbon). The Fe-NCNT with Fe-N 3 and FeNP exhibited a remarkably high specific activity (0.119 L min −1 m −2 ), which was 1.8 times higher than that of Fe-NCNT with only Fe-N 4 and obviously outperformed those of the state-of-the-art PMS activators. The low-coordinated structure and FeNP promoted the PMS reduction on Fe 2+ of Fe-N x for •OH and SO 4 •− production, which served as major oxidants for pollutants degradation . The experimental results and theoretical calculation corroborated the low-coordinated structure and FeNP jointly enhanced the PMS adsorption and electron density on Fe center, which accelerated electron transfer from Fe center to PMS for radical production.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Chinese Physics B
·
2020
·Vol. 29
·期 12
·127801
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IF 1.223
Yue Sun,Fenqi Du,Donghang Xie,Dongmei Yang,Yang Jiao,Lichao Jia,Haibo Fan
Iron (Fe) was successfully doped in CuWO4 photoanode films with a combined liquid-phase spin-coating method via the dopant sources of Fe(NO3)3, FeSO4 and FeCl3. The microstructure of the prepared films was characterized by x-ray diffraction, scanning electron microscopy, and atomic force microscopy. The light absorption and photoelectric conversion properties were evaluated by the UV-visible absorption spectra and monochromatic incident photon-to-electron conversion efficiency. The chemical composition and element combination of the samples were examined by x-ray photoelectron spectroscopy. A linear sweep voltammetric and stability test (I–t) were performed with an electrochemical workstation. The results show that the samples are uniform with a thickness of approximately 800 nm and that the photoelectrochemical performance of the doped films is heavily dependent on the Fe source and dopant concentration. Upon optimizing the doping conditions of Fe(NO3)3 and the optimal source, the photocurrent density in the Fe-doped CuWO4 photoanode film is improved by 78% from 0.267 mA/cm2 to 0.476 mA/cm2 at 1.23 V vs reversible hydrogen electrode. The underlying causes are discussed.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ke Lu,Mingyue Xia,Chaojun Chen,Hao Yuan,Jianping Liang,Hongli Wang,Zhi Zheng,Qinghua Liu,Junfeng Gao,Dezheng Yang
Plasma-synergistic catalysis is considered an effective method for degrading aromatic organic pollutants in water. However, the underlying synergistic catalytic mechanism between plasma and catalysts remains poorly understood. Here, we propose a plasma-metal organic frameworks (MOFs) synergistic strategy to investigate the mechanism of plasma-synergistic catalysts for phenol degradation. The results show that Fe-doped Zeolitic Imidazolate Framework-8 (Fe x -ZIF8, x = 0, 0.1, 0.2, 0.4) undergoes the plasma-induced transformation into an Fe-N 3 C structure (P-Fe-N 3 C), leading to a 4.5-fold enhancement in the phenol degradation rate compared to only plasma discharge. Density functional theory (DFT) calculations indicate that the plasma-induced structural transformation of Fe x -ZIF8 promotes the redistribution of point charges and space charges around the Fe center, thereby lowering the activation energy barrier in the rate-determining step (*C 6 H 4 (OH) 2 ). These findings not only provide theoretical support for the degradation of water pollutants via plasma-synergistic catalysts but also offer a novel strategy for constructing MOFs-derived materials.
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
研究领域:
环境科学
·
催化材料
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yuxiang Mao,Jun Cheng,Hao Guo,Lei Qian,Jiacan Tu,Weijuan Yang
To enhance catalytic acid-base sites in ZIFs and efficiently promote conversion of microalgal lipids, a bifunctional catalyst with single-atom Fe-N 4 sites and Fe nanoparticles (NPs) was synthesized by pyrolyzing Fe-doped ZIF-8. Compared with ZIF precursors, Fe nanoparticles and coordinated Fe ions in Fe-N 4 sites enhanced Lewis acidity, while increased uncoordinated N atoms enhanced Lewis basicity. Therefore, the acidity of Fe-NC increased from 0.473 to 1.845 mmol/g, while basicity increased from 0.172 to 0.439 mmol/g. DFT calculations showed that the adsorption energies of acetic acid on the Fe–N 4 and Fe NP were −0.536 eV and −0.397 eV, respectively, exceeding that (-0.190 eV) on the Zn–N 4 site. The energy barriers for rate-determining steps over the Fe-N 4 and Fe NP were + 0.32 eV and + 0.21 eV, respectively, which were lower than that (+1.01 eV) over the Zn-N 4 site. The maximum biodiesel yield reached 98.3% over Fe-NC catalyst, higher than that (84.5%) over ZIF-8 catalyst.
研究领域:
催化化学
·
能源材料
·
生物技术
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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
研究领域:
化学
·
材料科学
·
环境科学
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Wei Ding,Jing Xu,Tao Chen,Chengshuai Liu,Jinjun Li,Feng Wu
Previous studies have shown that the oxidation of Fe(II) by molecular oxygen can lead to the co-oxidation of As(III) at neutral pH. However, the mechanism of As(III) oxidation in the presence of Fe(II) with respect to the interaction between As(III) and Fe(II) is still unclear. In this work, we examined the oxidation of As(III) in the presence of Fe(II) in air-saturated water, which is affected by pH, co-existing phosphate, and scavengers ( tert -butanol, superoxide dismutase, catalase and dimethylsulfoxide). Results confirm that the formation of the Fe(II)–As(III) complex (formation constant, K Fe(II)–As(III) = 10 3.86 M –1 ) plays an extremely important role in the initial stage of As(III) oxidation at pH 7.25. The oxidation of Fe(II)–As(III) promotes the production of H 2 O 2 and colloidal ferric hydroxide. H 2 O 2 reacts with the Fe(II)–As(III) complex through oxidizing Fe(II) to Fe(IV), which then causes the partial oxidation (ca. 50%) of As(III). The other part of As(III) oxidation by H 2 O 2 occurs, in the form of Fe(III)–As(III) complex, through direct electron transfer from As(III) to H 2 O 2 but not through Fe(IV). This work provides new mechanistic insight into arsenic and iron redox chemistry in the environment and furthers our understanding of Fenton reactions at neutral pH.
研究领域:
环境化学
·
氧化还原化学
·
水处理
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产品关联
DOI
PubMed
高影响因子
HYDROMETALLURGY
·
2020
·
IF 3.338
Xintao Yi,Guangsheng Huo,Wei Tang
The extraction of Fe(III), Ni(II) and Co(II) from a Ni(II)-Co(II) solution containing Fe(III) was analyzed in a chloride medium using a mixed extractant consisting of 50% ( v /v) tributyl phosphate (TBP), 20% (v/v) 2-octanol and 30% (v/v) kerosene. The extraction of 0.5 mol/L Fe(III) in 4 mol/L hydrochloric acid reached 97%, and the consumption of chloride ions was investigated. Nickel(II) ions were not detectably extracted by TBP, with an inclusion of <1.1%. Compared with Fe(III), TBP extracted only a small amount of Co(II). The iron complexes formed by TBP and 2-octanol were [H 2 FeCl 4 · 2TBP] and [H 2 FeCl 4 · 5(2-octanol)], and the possible compositions of Co-containing extracts were [H 2 CoCl 4 · 2TBP] and [H 2 CoCl 4 ] · n[2-octanol]. An industrial process consisting of two-step extraction was designed to achieve the separation of Co(II) and Fe(III), resulting in a decrease in the Fe/Co mass ratio from 0.46 to <3.5 × 10 −4 in the raffinate.
研究领域:
化学工程
·
冶金学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zheng Wang,Keizo Nakagawa,Kecheng Guan,Aiwen Zhang,Yasunao Okamoto,Atsushi Matsuoka,Eiji Kamio,Tomohisa Yoshioka,Hideto Matsuyama
s The stability of solvent-resistant nanofiltration (SRNF) membranes, such as integrally skinned asymmetric (ISA) and thin-film composite (TFC) membranes, in polar aprotic solvents must be improved if they are to meet increasingly complex industrial demands. The stability of the former membranes can be improved by forming crosslinked rigid chains, such as polybenzimidazoles and polyimides, but this requires time-consuming treatment processes. Conversely, the latter membranes are easy to fabricate but lack efficient active sites for crosslinking and structural rigidity. Herein, we present a fabrication strategy combining the characteristics of both types of membranes. We first utilize amino-functional porphyrins as polyaromatic units to form rigid polyamide networks by vacuum-assisted interfacial polymerization, simultaneously providing active sites for further crosslinking, which is accomplished by immersion in FeCl 2 /dimethyl sulfoxide (DMSO) solution to directly establish Fe-O-Fe bridges between porphyrin centers to form a stable network. The Fe-O-Fe-bridged porphyrin networks are solvent-stable in DMSO. Furthermore, they achieve outstanding molecular separation (96.2% rejection of methyl orange, 327 Da) and limited molecular-weight-cutoff change (from 360 to 420 Da) during alternating MeOH and DMSO filtration, along with long-term recovery efficiency (> 96.7% over seven days). Thus, our study provides a promising strategy for the facile development and fabrication of efficient, robust SRNF membranes.
研究领域:
膜科学
·
材料工程
·
化学分离
·
高分子化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）