CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Xiaoli Zou,Tao Zhou,Juan Mao,Xiaohui Wu
In this study, a novel ultrasound-enhanced heterogeneous Fe 0 /persulfate (US/Fe 0 /PS) system was developed and investigated for the degradation of an antibiotic sulfadiazine (SD). It was demonstrated that the US/Fe 0 /PS system could achieve a significant synergy in the degradation efficiency of SD, as compared to its corresponding comparative systems. The SD degradation in the US/Fe 0 /PS system could be applied by the pseudo-first-order kinetic with a k obs (SD) value of 3.4 ± 0.20 h −1 . Affecting factors such as initial pH, dosage ratio of [Fe 0 ]:[PS], US input power and reaction temperature were further studied. SD could be effectively degraded with a relatively low PS dosage at a broad pH range of 3–7. Simultaneous evolution of soluble iron species and PS was evaluated in three comparative systems (US/Fe 0 , Fe 0 /PS and US/Fe 0 /PS) during the reaction. It could be concluded that the promotional role of US would be dual in the US/Fe 0 /PS system, i.e. enhancement in the heterogeneous iron corrosion reactions and acceleration in the bulk radical reactions. Identification of the degradation intermediates indicated that sulfate radical (SO 4 − ) oxidation was the main SD degradation pathway. Attacking of the amine group in the benzene ring would be its first step, followed by cleavage of C–N bonds in the heterocyclic ring. Another degradation pathway, i.e. direct cleavage of the S–N bond should be also present.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2017
·
IF 6.065
Weizhao Yin,Yongtao Li,Jinhua Wu,Guocai Chen,Gangbiao Jiang,Ping Li,Jingjing Gu,Hao Liang,Chuansheng Liu
A one-pot bio-iron system was established to investigate synergetic abiotic and biotic effects between iron and microorganisms on Cr(VI) removal. More diverse iron corrosion and reactive solids, such as green rusts, lepidocrocite and magnetite were found in the bio-iron system than in the Fe 0 -H 2 O system, leading to 4.3 times higher Cr(VI) removal efficiency in the bio-iron system than in the Fe 0 -H 2 O system. The cycling experiment also showed that the Cr(VI) removal capacity of Fe 0 in the bio-iron system was 12.4 times higher than that in the Fe 0 -H 2 O system. A 62 days of life-span could be achieved in the bio-iron system, while the Fe 0 -H 2 O system lost its efficacy after 30 days. Enhanced effects of extra Fe 2+ on Cr(VI) removal was observed, largely contributed to the adsorbed Fe 2+ on iron surface, which could function as an extra reductant for Cr(VI) and promote the electron transfer on the solid phase. The results also showed that the reduction of Cr(VI) by microorganisms was insignificant, indicating the adsorption/co-precipitation of Cr by iron oxides on iron surface was responsible for the overall Cr(VI) removal. Our study demonstrated that the bio-amended iron corrosion could improve the performance of Fe 0 for Cr(VI) removal from groundwater.
研究领域:
环境科学
·
微生物学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Longqian Wang,Jingya ye,Jingyi Zhang,Qinglong Meng,Xiaoyu Li,Zhonglin Chen,Huahu Yu,Ao Zhang,Zhuoyu Bu,Yongli Jiao,Yuwei Pan
Peracetic acid (PAA) was successfully activated by UV and Fe 0 to degrade sulfamethazine (SMT) in this study. UV/Fe 0 /PAA system not only could enhance SMT removal efficiency but also could reduce the energy consumption in comparison with UV, Fe 0 /PAA and UV/PAA systems. The R O • radical was the main radical for the degradation of SMT in UV/Fe 0 /PAA system and photolysis, • OH and R-O • exhibited 15.6%, 17.6% and 66.8% contribution for SMT degradation, respectively. Fourier transform infrared spectroscopy (FTIR), Scanning Electron Microscope (SEM), and X-ray photoelectron spectroscopy (XPS) were conducted to investigate the characterization of Fe 0 after reaction in UV/Fe 0 /PAA system. The possible SMT degradation pathway was also proposed. Affecting factors such as Fe 0 dosage (0–0.2 g L −1 ), PAA concentration (0–200 μM) and initial pH (3–9) were also studied. Cl − , NO 3 - , SO 4 2- and HCO 3 - had a negligible adverse effect on SMT removal in this system indicating the good adaptability to inorganic ions. In addition, UV/Fe 0 /PAA system had the good recycle ability of Fe 0 and showed a good performance in removing antibiotic in the nature fresh water. Therefore, this study notably improved the knowledge of PAA activated by Fe 0 and UV and showed the potential applicability of UV/Fe 0 /PAA system in degrading antibiotics in nature fresh water.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2019
·Vol. 79
·期 7
·1287-1296
·
IF 1.624
Liu Yunxin,Zhou Peng,Huo Xiaowei,Liu Yang,Cheng Xin,Zhang Yongli
Our findings proved that micron-scale zero-valent iron (mZVI) particles with pre-magnetization combined with peroxymonosulfate (PMS) can markedly enhance the removal of acid orange 7 (AO7). Investigation into the mechanism showed that PMS accelerated the corrosion of ZVI to release Fe 2+ under acidic conditions, and the in-situ generated Fe 2+ further activated PMS to produce SO 4 • − and •OH, resulting in AO7 removal. Further, the Lorentz force strengthened the convection in the solution and the field gradient force tended to move Fe 2+ from a higher to a lower field gradient at the pre-magnetized ZVI (Pre-ZVI) particle surfaces, thus indicating that pre-magnetization promoted the corrosion of ZVI to release Fe 2+ , which resulted in the enhancement of PMS activation. Nano-scale ZVI (nZVI) was more effective than mZVI in activating PMS to degrade AO7, but the pre-magnetization effect on mZVI was better than on nZVI. AO7 removal increased with higher ZVI and PMS dosage, lower AO7 concentration, and acidic conditions (pH = 2, 3). This study helps to understand the reactive radicals-based oxidation process with application of pre-magnetized ZVI in activating PMS.
研究领域:
环境化学
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高级氧化技术
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水处理
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2017
·
IF 6.942
Haoxuan Li,Yili Wang,Huaili Zheng
The feasibility of using Fe 0 /S 2 O 8 2− conditioning (zero valence iron (ZVI)/persulfate (ps)) integrated with horizontal electro-dewatering (HED) to improve the dewaterability of activated sludge (AS) was evaluated. The removal and migration of free and bound water in the ZVI/ps–HED process were determined, along with the organic matter migration between the solid and liquid phases of AS biosolids . Results showed that the optimum conditioning dosages were determined as 0.35 g ZVI/g dry solids (DS) and 0.15 g ps/g DS on the basis of capillary suction time variation. The lowest final water content (WC) of 83.67% in AS occurred after the HED treatment at 40 V and 120 min as determined using the response surface methodology . Despite the disruption of AS flocs and microbial cells through SO 4 − · oxidation during the ZVI/ps conditioning, the particle size and mass fractal dimension of the AS flocs remained relatively stable as the zeta potential increased from −8.5 mV to −4.6 mV. The coagulation of Fe 3+ from the oxidation of Fe 2+ by ps contributed to the relatively stable condition, which favored the subsequent momentum of the electroosmotic flow. Moreover, the ZVI/ps conditioning decreased the bound water content (BWC, from 1.83 g/g DS to 1.38 g/g DS) and increased the free water content (FWC, from 60.27 g/g DS to 60.91 g/g DS), indicating a transformation from free water to bound water. After the ZVI/ps–HED process, the FWC and BWC were removed significantly with ratios of 96.32% and 79.78%, respectively. Along with water removal through the ZVI/ps–HED process, the organic matter in the supernatant/filtrate initially increased and further rose at the HED stage. The analysis of the extracellular polymeric substance (EPS) content showed that the proteins (PNs) and polysaccharides (PSs) at the liquid and solid phases decreased due to oxidative degradation. Furthermore, the ZVI/ps stage significantly reduced the PNs content of slime to 57.22%, the PSs content of EPS to 68.50%, and the PN-like substances in the slime and tightly bound EPS to 74.90% and 52.47%, respectively. In addition, the WC of AS correlated with the contents of PN and microbial by-product-like material in slime, as well as tryptophan in TB-EPS, and the low EPS content in AS indicated good dewaterability. Thus, ZVI/ps should be selected as a pretreatment prior to HED.
研究领域:
环境科学
·
污水处理
✓ 已验证
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Qin Hejie,Yang Han,Zhang Zhenmin,Feng Yiran,Sun Yuankui,Fan Peng,Ao Zhimin,Waite T. David,Guan Xiaohong
Perchlorate (ClO 4 − ) contamination in water poses global health risks, yet its efficient reduction to harmless Cl − under mild conditions remains challenging. Here, we report a donor−acceptor catalytic system comprising defective MoS 2 on N-doped carbon (MoS 2 −NC) coupled with zerovalent iron (Fe 0 ), which enables rapid ClO 4 − reduction at near-neutral pH (rate constant, 2.36 h −1 ), yielding Cl − as the sole product. In the MoS 2 −NC/Fe 0 system, Fe 0 acts as the electron donor, while undercoordinated Mo atoms in defective MoS 2 serve as the active sites, and N-doped carbon mediates electron transfer and optimizes the electronic environment for ClO 4 − reduction. The reduction proceeds via oxygen atom transfer, involving Cl−O bond cleavage, O binding to Mo sites, and hydrodeoxygenation of the Mo-bound O atoms. Our observations offer a practical strategy for ClO 4 − reduction without harsh conditions or noble metals and underscore the promise of donor−acceptor-based, defect-engineered catalysts for reductive transformation of challenging oxyanions.
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jia-Qi Zhou,Huan-Yan Xu,Bo Li,Bao-Ying Wang,Yue Liu,Zhi-hao Zhao,Yan-Li Zhuang
Achieving the harmless degradation of organic pollutants remains a challenging task for the advanced oxidation processes. Metal-organic frameworks have emerged in the field of energy and environmental catalysis. Herein, MIL-101(Fe) was employed as the precursor to prepare a porous carbon embedded Fe 0 nanoparticles (Fe 0 @C) via a pyrolytic process under N 2 protection. MIL-101(Fe) and Fe 0 @C were characterized in detail by various instrumental techniques. The control experiments indicated that Fe 0 @C exhibited much higher capacity to activate peroxymonosulfate (PMS) for the degradation of Levofloxacin (LEV) than MIL-101(Fe). Within 60 min reaction time, LEV degradation efficiency was increased from 37.0% in the MIL-101(Fe)/PMS system to 96.3% in the Fe 0 @C/PMS one. The affecting parameters of Fe 0 @C/PMS system were investigated systematically, including LEV concentration, Fe 0 @C dosage, PMS dosage, solution pH and coexisting anions. Furthermore, various representative organic pollutants could be efficiently degraded in the Fe 0 @C/PMS system. Radical quenching tests and electron paramagnetic resonance (EPR) disclosed that singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 •- ) and hydroxyl radical (•OH) governed the degradation of LEV, among which 1 O 2 played the most prominent role. Meanwhile, the degradation intermediates and pathways of LEV under the radical and non-radical attacks were deduced by high-performance liquid chromatography-quadrupole-time of flight mass spectrometry (HPLC-QTOF/MS) assisted by density functional theory (DFT) calculations. The reasonably designed Fe 0 @C might facilitate electron transfer and thus promote Fe(III)/Fe(II) cycle and PMS activation. This work will provide a new idea for the development of MOFs-derived carbon-based persulfate activators.
研究领域:
环境科学
·
催化化学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ruoyu Deng,Qiang He,Dongxu Yang,Qi Dong,Jiali Wu,Xiangyu Yang,Yi Chen
Dielectric barrier discharge (DBD) is an attractive advanced oxidation process (AOP) due to its operational convenience and environmental friendliness. However, DBD plasma suffers from relatively low energy utilization, which limits its commercial application. In this study, nano-Fe 0 -CeO 2 is successfully synthesized and used for DBD plasma degradation of diclofenac (DCF). The results show that the nano-Fe 0 -CeO 2 significantly enhances the removal of DCF. A DBD-Fe 0 -CeO 2 system degrades 96.4% DCF within 10 min, which is higher than the DBD system alone (45.8%). The synergistic factor of the DBD system and nano-Fe 0 -CeO 2 reaches 3.731. In addition, the composite catalyst shows ideal reusability. Substance activity and production experiments show that reactive oxygen species (ROS), especially OH, play a key role in the degradation of DCF. Nano-Fe 0 -CeO 2 has synergistic effects with O 3 and H 2 O 2 and significantly promotes the generation of ROS in the DBD system. Based on the intermediates detected by liquid chromatography-mass spectrometry, a reasonable degradation pathway of DCF is proposed. Our findings are helpful for understanding the mechanism of DCF degradation by coupling nano-zero-valent-iron-based nanocomposites in a DBD system; they also provide an effective system for the treatment of refractory organic pollutants in water.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2021
·Vol. 232
·期 3
·1-14
·
IF 2.52
Pan Yuwei,Bu Zhuoyu,Li Xiang,Han Jiangang
This study presented the efficient removal of tartrazine, a typical biorefractory dye, in a heterogeneous photochemical Fenton-like system adopting Fe 0 and oxalate (Ox) (UV/Fe 0 /Ox). Only 47.4% tartrazine could be removed within 60 min with a UV/Fe 0 system. The addition of Ox could significantly enhance the removal of tartrazine to 72.4% within only 20 min with the UV/Fe 0 /Ox system. The effects of various factors, such as the Fe 0 dose (0–0.8 g/L), Ox dose (0–2 mM), initial pH (2–6), and initial tartrazine concentration (2–30 mg/L), on the removal of tartrazine were examined. Scanning electron microscopy (SEM), Fourier transform infrared (FTIR) spectroscopy, and Mossbauer spectroscopy were conducted to explore the mechanism by which oxalate enhances the performance of the UV/Fe 0 system. Ox could inhibit the formation of iron (hydro)xides on the Fe 0 surface, thus guaranteeing the reactivity of Fe 0 during the reaction. Compared with Fe 2 O 3 , FeS, and Fe 3 O 4 , Fe 0 was a good heterogeneous iron catalyst for the photolysis of tartrazine with the Ox system. Compared with H 3 PO 4 , nitrilotriacetic acid, and ethylenediaminetetraacetic acid, Ox was also a good photolysis chelating agent. The UV/Fe 0 /Ox system could also maintain fast tartrazine removal after five consecutive runs without the addition of Fe 0 , indicating the good stability of Fe 0 .
研究领域:
环境科学
·
化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Rui Li,Haoran Dong,Ran Tian,Jie Chen,Qianqian Xie
In this work, bare nanoscale zero-valent iron (NZVI) and the modified NZVI (sulfide-modified NZVI, Ni/NZVI and activated carbon supported NZVI) were utilized to activate sulfite for the removal of the target pollutant sulfamethazine (SMT). Some critical factors influencing the removal process were investigated, including dosage of sulfite and nanoparticles (NPs), ratios of modifier/NZVI, dissolved oxygen, initial pH values, groundwater components and aging time of NPs. Under the optimal conditions, in terms of the dosage of sulfite/NPs and the ratio of modifier/NZVI, all the modified NZVI showed a better performance than the bare NZVI. Dissolved oxygen was determined to be an essential factor for producing reactive radicals in all the activation processes. The active radicals were identified to be SO 4 · and HO·, and HO· was evidenced as the principal reactive species. Initial pH value significantly affected the SMT removal, which was obviously inhibited under alkaline condition. In such case, Ni/NZVI showed a better performance than the other NPs due to the catalysis effect of Ni. It was also found that the groundwater components (e.g., HCO 3 − , Ca 2+ , SO 4 2− , and humic acid) could restrain the removal process because of the buffering effect, the radical scavenging effect and some other effects (e.g., surface precipitation). Spectroscopic analysis of the fresh and aged (30 d) NPs illustrated that both bare and modified NZVI were slightly oxidized in the air, and could still be employed for the activation of sulfite.
研究领域:
环境科学
·
水处理
·
纳米技术
·
污染物去除
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Miaoqing Li,Rui Luo,Chaohai Wang,Ming Zhang,Wuxiang Zhang,Prosper Kwame Klu,Yubo Yan,Junwen Qi,Xiuyun Sun,Lianjun Wang,Jiansheng Li
The rational design of active and sustainable heterogeneous catalysts towards advanced oxidation process (AOPs) is of great significance for water remediation. Here, we synthesized Fe 0 /graphitized carbon composite catalysts for efficient removal of bisphenol A (BPA) by activating peroxymonosulfate (PMS). The Fe 0 /graphitized carbon composites were obtained by the pyrolysis of iron-tannic modified cotton, where tannic acid (TA) is an eco-friendly and low-cost polyphenol that can strongly form complexes with iron ions. The introduction of iron could significantly regulate the graphitization of carbon by changing the pyrolysis temperature. The combination of Fe 0 and graphitized carbon can endow Fe-TCs with an enhanced adsorption ability due to strong complexation between Fe 0 and BPA. The pyrolysis of iron-tannic modified cotton may serve as a novel strategy to design an efficient low-toxic metal-carbon catalyst for sulfate radical based processes in water remediation.
研究领域:
环境科学
·
材料科学
·
化学工程
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Fa Fang,Nuo Li,Xian Zhang,Juan Liu,Jingzi Beiyuan,Jielong Cao,Jin Wang,Yanyi Liu,Gang Song,Tangfu Xiao
Due to extreme toxicity of the element of thallium (Tl), increasing aqueous Tl pollution incidents have aroused growing concerns. As the prevalent and stable form, i.e. , monovalent Tl, the highly efficient removal methodologies of Tl(I) from (waste)water remains limited and challenging. In this study, an advanced oxidation method, the feasibility of using zero valent iron (Fe 0 ) coupled with persulfate (PS) to treat Tl(I)-containing synthetic wastewater was investigated. Its influence parameters, including reaction time, initial Tl concentration, dosages of PS and Fe 0 , initial and coagulation pH, temperature, coexisting ions and organic matter (NO 3 − , SO 4 2− , Cl − and HA) were examined. The results revealed that the system can be applied to a wide range of pH and temperature and the reaction equilibrium can be reached in about 30 min. Favorable Tl(I) removal rate (>98%) was observed in the synthetic wastewater with medium and relatively high Tl(I) concentration (≤0.250 mM). The analyses of characterization results including electron spin resonance spectrometer and X-ray photoelectron spectroscopy indicated that ·OH played a vital role in the removal of Tl(I), which was oxidized and removed by co-precipitation. Fe 0 can be served as a stable source of Fe 2+ to efficiently catalyze PS. The remaining Fe 0 can be easily separated because of its magnetism, assuring the promising reusability of the reactant. The study aims to provide references for treatment of real Tl polluted wastewater.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）