ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Fanxu Meng,Jiang Xu,Huiwang Dai,Yunlong Yu,Daohui Lin
Surface modification of microscale Fe powder with nitrogen has emerged recently to improve the reactivity of Fe0 for dechlorination. However, it is unclear how an even incorporation of a crystalline iron nitride phase into Fe0 nanoparticles affects their physicochemical properties and performance, or if Fe0 nanoparticles with a varied nitridation degree will act differently. Here, we synthesized nitridated Fe0 nanoparticles with an even distribution of N via a sol–gel and pyrolysis method. Nitridation expanded the Fe0 lattice and provided the Fe4N species, making the materials more hydrophobic and accelerating the electron transfer, compared to un-nitridated Fe0. These properties well explain their reactivity and selectivity toward trichloroethylene (TCE). The TCE degradation rate by nitridated Fe0 (up to 4.8 × 10–2 L m–2 h–1) was much higher (up to 27-fold) than that by un-nitridated Fe0, depending on the nitridation degree. The materials maintained a high electron efficiency (87–95%) due to the greatly suppressed water reactivity (109–127 times lower than un-nitridated Fe0). Acetylene was accumulated as the major product of TCE dechlorination via β-elimination. These findings suggest that the nitridation of Fe0 nanoparticles can change the materials’ physicochemical properties, providing high reactivity and selectivity toward chlorinated contaminants for in situ groundwater remediation.
研究领域:
环境科学
·
纳米材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zishen Lin,Chunli Zheng,Zhenxing Wang,Yuanzhe Peng,Guoqing Geng,Aibin Zhu,Chi He
As one category of promising and efficacious purification material toward environmentally harmful heavy metals, sulfidated amorphous zero-valent Iron (S@AZVI) exhibits unparalleled removal performance. Due to the disruptive crystal growth however, the irreversible loss of Fe 0 component during conventional synthesis route poses a substantial hindrance to its industrial application. To address this, we propose a post-sulfidation strategy to hinder the transformation of Fe 0 by altering the shell composition of AZVI from Fe 2 O 3 to FeS, which maintains a remarkable Fe 0 content up to 75.7 % over finally obtained S@AZVI, far higher than the material obtained through the one-step sulfidation . Attributing to the synergy of FeS shell and substantial Fe 0 , S@AZVI demonstrates impressive performance as the lowest free corrosion potential (−1.050 V) and work function (4.058 eV), and subsequently exhibits a notable enhancement in the removal efficiency of Cr(VI) and Ni(II), surpassing AZVI by 1.8 and 2.0 times, respectively. Results reveal that the adsorption, reduction, and coprecipitation constitute the mechanisms governing the removal of Cr(VI) and Ni(II). In practical electroplating wastewater experiments, S@AZVI effectively removes Cr(VI) and Ni(II) within a 60-min timeframe, meeting established emission standards. These findings provide valuable insights for future AZVI material synthesis for heavy metal elimination.
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
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Xiangyu Wang,Anqi Wang,Mengyang Lu,Jun Ma
Novel ternary nanocomposite based on nano zero-valent iron (nZVI) and graphene-TiO 2 nanowires (Fe@GNW) was successfully synthesized for both reduction and photocatalytic oxidation of metronidazole (MNZ). Fe@GNW exhibits synergetic effects and significant properties, such as facilitating the photogenerated charges separation, enhancing the surface activity of nZVI, improving the adsorbent ability of catalyst, possessing the magnetic property for facile recycling. Due to the formation of micro-graphene-nZVI batteries and heterogeneous photo-Fenton system, Fe@GNW showed a superior activity in removal of MNZ (99.3%) compared with TiO 2 nanowires (43.0%) and graphene-TiO 2 nanowires (67.6%). Moreover, Fe@GNW retained excellent stability without apparent loss in catalytic activity after five cycles. MNZ removal by Fe@GNW experienced a two-stage process of reduction-adsorption and photocatalytic oxidation, which could be well-described by a revised pseudo-first order kinetics. The decomposition pathways of MNZ were proposed based on the analysis of intermediates. The quenching tests demonstrated that h + and OH are responsible for MNZ decomposition. New insights into the mechanism of the enhanced reduction and photodegradation of MNZ were proposed.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2015
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IF 7.435
Tao Zhou,Xiaoli Zou,Juan Mao,Xiaohui Wu
Effective decomposition of antibiotic sulfadiazine (SD) in a Fe 0 -catalyzed sonochemical Fenton like system (Sono-FL) was demonstrated. By using the response surface methodology (RSM), an optimized experimental condition of pH 7.00, 0.94 mM Fe 0 , 1.90 mM persulfate (PS) and 20 W ultrasound (US) power was concluded, which could reach the predicted SD degradation efficiency of 90%. Afterwards, effects of wastewater matrix (five inorganic anions and two chelating agents) on the SD degradation were investigated in the system, respectively. It was found that the SD degradation could be inhibited by SO 4 2− , NO 3 − , HCO 3 − /CO 3 2− and H 2 PO 4 − to different extents. Cl − would lead to an enhancement with a low dosage (5 mM), but an inhibition with a high dosage (100 mM). Unexpectedly, chlorinated organic intermediates were also found as SD decomposed. Appropriate dosages of oxalic acid (OxA) or EDTA could benefit the SD degradation in the Sono-FL system, while excessive chelating agents would play as competitive pollutants. It was summarized that inorganic anions would mainly react with SO 4 − and/or OH to form sub-radicals of less oxidative potential. OxA and EDTA would not only participate in complexing dissolution of Fe 0 but also provide additional oxidants such as H 2 O 2 and [Fe IV O] 2+ , through the electron transfer reactions caused by the iron-ligands species.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Dongmei Ma,Jing Wang,Kun Feng,Bingfeng Liu,Guojun Xie,Defeng Xing
Zerovalent iron (Fe 0 )-based biochar (Fe 0 -BC) has attracted wide attention in activating persulfate to eliminate antibiotics. In this study, the waste red mud (RM) was successfully used as an iron precursor to prepare Fe 0 -BC (RMIS 1:1 ) via co-pyrolysis strategy, which was confirmed with remarkable capacity in peroxydisulfate (PDS) activation. The removal efficiency of sulfadiazine (SDZ) was 99.7% in RMIS 1:1 /PDS system in 20 min, with k obs of 0.3001 min −1 . Both free radicals (SO 4 − , OH, and O 2 − ) and non-free radicals ( 1 O 2 ) were responsible for SDZ degradation, in which the SO 4 − and O 2 − played the dominant roles. Four SDZ degradation pathways were provided according to the intermediates identified by Q-TOF-MS. Furthermore, the ECOSAR prediction implied that the intermediates have less eco-toxicity than SDZ. Compared with PDS concentration and RMIS 1:1 dosage, the initial SDZ concentration had stronger effect on its degradation. Co-existed Cl − slightly improved SDZ degradation rate, while other anions (NO 3 – /SO 4 2− /HCO 3 – /CO 3 2– ) and humic acid exhibited different levels of inhibition on SDZ removal. Moreover, RMIS 1:1 /PDS maintained acceptable degradation ability for practical pharmaceutical wastewater. The electrical energy per mass of SDZ was about 2.24 kWh/(g·SDZ) by RMIS 1:1 /PDS, lower than that produced in any other advanced oxidation processes that have been reported so far. In summary, this study reported a green strategy for Fe 0 -BC preparation from RM, which was valuable for both waste resource recycling and environmental remediation.
研究领域:
环境科学
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废弃物资源化
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污染治理
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DOI
高影响因子
WATER AIR AND SOIL POLLUTION
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2022
·Vol. 233
·期 12
·1-14
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IF 2.984
Li Weiquan,Li Mingxi,Yin Weizhao,Zhang Weinan,Zhong Jiawei,Li Ping,Deng Hong,Wu Jinhua
The removal of Cr(VI) from groundwater by zero-valent iron (Fe 0 ) and microorganisms under different nutrients and electron-accepting conditions was investigated using continuously-flowed column reactors with an abiotic Fe 0 column as the control. Both abiotic and biotic Fe 0 columns were operated at low and relatively high concentrations of organic substrates (sodium acetate and humic acid) and electron acceptors (nitrate and sulfate). Sodium acetate and humic acid were found to be effective substrates for the biotic Fe 0 system to remove Cr(VI) since microorganisms were able to gain extra reducing capacity from two nutrients and simultaneously avoid the passivation effect of humic acid on Fe 0 by metabolizing it. For nitrate and sulfate, varied influences were observed in the biotic Fe 0 system. The former showed apparent inhibition on Cr(VI) removal as it competed with Cr(VI) for electrons, and the inhibition became more severe while nitrate concentrations increased. Differently, highly reactive minerals such as green rusts and iron sulfide could be generated on the biotic Fe 0 surface under sulfate-reducing condition. They significantly enhanced Cr(VI) removal by providing more adsorptive and reductive sites. Overall, though the biotic Fe 0 column exhibited a longer life-span and higher Cr(VI) removal capacity than the abiotic Fe 0 column, the effects of organic substrates and electron acceptors should still be taken into account when applying biotic Fe 0 systems for Cr(VI)-contaminated groundwater remediation.
研究领域:
环境科学
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微生物学
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DOI
高影响因子
CHEMOSPHERE
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2023
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IF 8.8
Bin Li,Chen-Xuan Li,Yan Wang,Weiyi Xu,Kangping Cui,Xinyuan Zhan,Rui Deng,Xing Zhang
Nano zero-valent iron (nZVI) is extensively used as a peroxymonosulfate (PMS) activator but suffers from the ease of oxidation and agglomeration due to its high surface energy and inherent magnetism. Here, green and sustainable yeast was selected as a support material to firstly in-situ prepare yeast-supported Fe 0 @Fe 2 O 3 and used for activating PMS to degrade tetracycline hydrochloride (TCH), one of the common antibiotics. Due to the anti-oxidation ability of the Fe 2 O 3 shell and the support effect of yeast, the prepared Fe 0 @Fe 2 O 3 /YC exhibited a superior catalytic activity for the removal of TCH as well as some other typical refractory contaminants. The chemical quenching experiments and EPR results demonstrated SO 4 •− was the main reactive oxygen species while O 2 •− , 1 O 2 and • OH played a minor role. Importantly, the crucial role of the Fe 2+ /Fe 3+ cycle promoted by the Fe 0 core and surface iron hydroxyl species in PMS activation was elucidated in detail. The TCH degradation pathways were proposed by LC-MS and density functional theory (DFT) calculation. In addition, the outstanding magnetic separation property, anti-oxidation ability, and high environmental resistance of the catalyst were demonstrated. Our work may inspire the development of green, efficient, and robust nZVI-based materials for wastewater treatment .
研究领域:
环境科学
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催化化学
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废水处理
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xiaonan Hu,Yang Ye,Gang Lu,Gang Ren,Chuanyi Wang,Mingshan Zhu
To tackle high salinity challenge, differently from singlet oxygen-governed systems, extremely abundant and highly reactive sulfate radicals (SO 4 •─ )-dominated systems might be also feasible. Ingenious integration of two active popular catalysts, and optimal selection of reaction parameters could sufficiently activate the added peroxymonosulfate (PMS) to efficiently degrade complicated pollutants within a short time so as to overlook the negative effects of inorganic anions. Herein, zero-valent iron decorated metallic 1T/semiconducting 2H hybrid phased molybdenum disulfide with different Mo/S feeding ratio (Fe 0 /Nx-MoS 2 ) were constructed and compared to activate PMS for carbamazepine (CBZ) removal, where Fe 0 /N2-MoS 2 (M(Mo):M(S) = 7:30) with ultrathin sheet morphology presented most charming decontamination performance. Optimal Fe 0 /N2-MoS 2 dosage and PMS amount was respectively selected as 75 and 50 mg·L -1 in treating 10 mg·L -1 CBZ at pH = 3.00 via tailoring reaction parameters. CBZ could be completely removed in a short time of 10 min with a high pseudo-first-order kinetic rate constant of 0.939 ± 0.016 min −1 . The system exhibits the promising anti-interference capacity toward Cl ─ , NO 3 ─ and SO 4 2─ of high concentration (even up to 3000 mg·L -1 ). Electron paramagnetic resonance and scavenging experiments of reactive species suggested that SO 4 •─ played a dominant function. Furthermore, Mo and Fe bimetallic cycles could efficiently promote PMS activation to produce rich reactive radicals. Degradation pathways and toxicity evolutions for CBZ in the (Fe 0 /N2-MoS 2 + PMS) system were proposed via liquid chromatography time-of-flight mass spectrometer and Toxicity Estimation Software Tool, and we hope that the system would be applied in high salinity wastewater treatment in future.
研究领域:
环境科学
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催化化学
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水处理工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ali Shan,Usman Farooq,Shuguang Lyu,Waqas Qamar Zaman,Zain Abbas,Meesam Ali,Ayesha Idrees,Ping Tang,Ming Li,Yong Sun,Qian Sui
Trichloroethylene (TCE) is chloride organic solvent used in industrial process and frequently detected as one of contaminants in groundwater. In present study, nano zero valent iron-nickel composite (nZVI-Ni) was prepared successfully by ion exchange process and investigated as a proficient sodium persulfate (SPS) activator for the removal of TCE in Fenton-like oxidation system. The physico-chemical characteristics, structure, and surface morphology of the prepared nZVI-Ni nanocomposite was analyzed through energy dispersive spectroscopy (EDS), scanning electron microscopy (SEM), N 2 adsorption-desorption, transition electron microscopy (TEM), X-ray diffractometry (XRD) and X-ray photoelectron spectroscopy (XPS). The experimental results obtained from batch tests in lab showed that more than 95% of TCE could be removed efficiently at nZVI-Ni/SPS/TCE molar ratio of 4/4/1 within 120 min at 20 °C. Further scavenging tests were designed to examine the presence of HO , SO 4 − and O 2 − radicals and verified the major role of HO radical in the nZVI-Ni/SPS system for the complete removal of TCE. Moreover, the generation of HO radicals in the system was confirmed through electrons paramagnetic resonance (EPR) of nZVI-Ni composite. The influence of surfactants on TCE removal was tested and the results showed that the percentage removal of TCE was recorded as 97.75%, 95.63% and 77.50% in the presence of Tween-80, BRIJ-35 and TX-100 surfactants at the nZVI-Ni/SPS/TCE molar ratio of 80/80/1, respectively. Results of TCE degradation in real groundwater revealed that nZVI-Ni can be applicable and is a promising catalyst for TCE removal in in-situ chemical oxidation (ISCO) practice. In Summary, these significant findings strongly demonstrate the feasibility and potential of nZVI-Ni activated SPS process as an alternative technique for TCE contaminated groundwater remediation.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
·
IF 8.4
Ruofan Wu,Xu Zhai,Zhenli He,Xiaoe Yang
Elevated concentrations of nitrite (NO 2 − ) in water pose considerable health risks, including methemoglobinemia and carcinogenesis, yet this issue has been relatively underexplored. This study successfully synthesized Fe-N co-doped carbon (Fe 3 C@Fe-CN-3) by incorporating iron carbide (Fe 3 C) and Fe 0 into N-doped carbon, thereby enhancing the activation of peroxydisulfate (PS) for NO 2 − removal. The impacts of diverse materials and the experimental parameters (different initial pH, PS concentration and ions) on activation efficiency were investigated. The results demonstrate that a molar ratio (1.2) of Fe to N in the raw material led to the formation of Fe 3 C, whereas reducing this ratio to 0.8 resulted in the formation of iron nitride (Fe 4 N). Fe 3 C@Fe-CN-3, synthesized with a molar ratio of 1.2, exhibited the highest removal rate of NO 2 − (73.8 %) at a PS concentration of only 0.2 mM, with a rate constant (K obs ) of 0.049 min −1 . To achieve a basic NO 2 − removal rate (99.5 %), a molar ratio of at least 7:20 between NO 2 − and PS is required. The non-radical pathway involved in NO 2 − removal was confirmed through delayed experiments and electron suppression tests. Meanwhile, Electron paramagnetic resonance (EPR) and radical scavenging experiments confirmed that hydroxyl radicals ( O H · ) and superoxide anion radicals ( O 2 − · ) play key roles in the removal process. While Fe 3 C@Fe-CN-3 showed excellent reusability, the removal rate was significantly reduced when natural water was employed as the reaction medium, emphasizing the imperative to enhance its selective removal capabilities.
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jiayan Zhu,Lishan Zhang,Junyong Liu,Shan Zhong,Zengxian Wei,Pin Gao,Jinyou Shen
In this study, we present a novel approach to fabricate a granular ceramic material utilizing a composite of nano zero-valent iron (nZVI), carbon, and kaolin. The optimal mass ratio of the prepared material was kaolin, nZVI, activated carbon, and appropriate additives = 40%:40%:10%:10%. The resulting composite demonstrated microelectrolysis effects, enhancing its reactivity for pollutant removal. Activated carbon within the composite significantly increased the interlayer spacing of kaolin, and improved material performance. Furthermore, the addition of activated carbon proved effective in preventing the agglomeration of nZVI, and ensuring a stable and efficient pollutant removal process. The results of 40-day column experiments showed that nano iron-carbon-kaolin micro-electrolysis particles (NIMP) consistently demonstrated stable trichloroethane (TCE) removal with an average removal rate of 88.15 ± 3.24%. Batch experiments confirmed that the synthesized material can achieve complete dechlorination of TCE, which was consistent with density functional theory calculations. The developed material exhibited a robust soil structure and high reactivity for pollutant reduction, making it a promising substrate filler for efficiently degrading refractory organic pollutants. It holds great potential for applications in areas such as water treatment and soil remediation.
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
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Wuming Xie,Zijun Huang,Fengping Zhou,Yuhui Li,Xiaolin Bi,Qiushi Bian,Shuiyu Sun
The presence of the antibiotics in wastewater and drinking water is causing increasing concern around the world, thereby an advanced sustainable technology needs to be developed to remove the antibiotics from water resources. In this study, Metal-organic frameworks (MOFs) derived zero-valent iron embedded in the carbon matrix structure named FMC is prepared by a direct pyrolysis of Fe-based metal organic framework. FMC is used as a heterogeneous Fenton-like catalyst to degrade amoxicillin (AMX) based on the oxidation and degradation reactions. FMC had the strengthened catalytic performance for amoxicillin elimination with high mineralization efficiency (60.41%), which was evaluated over various experimental conditions. The role of reaction in FMC/H 2 O 2 system was identified, suggesting amoxicillin was eliminated by the attack of hydroxyls radicals (·OH). The carbon structures can facilitate the passage of electrons and boost the contact of zero valent iron and Fe 2+ species on FMC surface with H 2 O 2 , resulting in the accelerated production of ·OH and high removal efficiency of amoxicillin. By defining reactive oxidizing species and degradation intermediates, the plausible degradation pathways of amoxicillin have been inferred. This study revealed that FMC/H 2 O 2 system has high AMX degradation efficiency and decent recyclability .
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
高影响因子
危险品化学品经营许可证（带存储）