SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Huidi Zhang,Yao Deng,Junhui Yang,Jinglin Yin,Jing Wang,Hongbo Xiao,Lizhi Wang,Cuihong Zhang,Wenlei Wang
In this study, MnPc intercalated Zn/Fe layered double hydroxides (MnPc/ZF−LDH) were synthesized by pillared intercalation modification with different MnPc intercalation amounts and used for the selective transformation and removal of As(III) from the arsenate-phosphate mixed solution. Fe−N bonds were constructed by the complexation of MnPc and iron ions on the Zn/Fe layered double hydroxides (ZF−LDH) interface. The DFT calculation results show that the binding energy of Fe−N bonded to arsenite (−3.75 eV) was higher than that of phosphate (−3.16 eV), resulting in MnPc/ZnFe−LDH exhibiting high As(III) selective adsorption performance and anchoring it rapidly in the arsenite -phosphate mixed solution. The maximum adsorption capacity of 1MnPc/ZF−LDH for As(III) could reach 180.7 mg·g −1 under dark conditions. MnPc also acts as a photosensitizer to provide more active species for the photocatalytic reaction. A series of experiments demonstrated that MnPc/ZF−LDH exhibits high As(III) selective photocatalytic performance. A total of 10 mg·L −1 of As(III) was completely removed in the reaction system within 50 min in a single As(III) environment. In an environment with As(III) and PO 4 3− , it achieved 80.0 % removal efficiency of As(III) and showed a good reuse effect. The introduction of MnPc could improve the utilization of visible light by the MnPc/ZnFe−LDH. The singlet oxygen generated from photoexciting MnPc leads to abundant ZnFe−LDH interface OH. In addition, MnPc/ZnFe−LDH shows good recyclability , making it a promising multifunctional material for the purification of arsenic-polluted sewage.
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jinyuan Zhu,Lu Wang,Waseem Hayat,Yongqing Zhang,Shaobin Huang,Xinfeng Zhang,Shaoqi Zhou
The abundant and environmentally friendly metal iron (Fe) is an excellent candidate to activate peroxymonosulfate (PMS) for the oxidative decomposition of organic pollutants . However, Fe-based activators have disadvantages of high efficiency only in a narrow pH range and easily generated Fe-sludge. Therefore, developing wide pH range efficient and stable Fe-based PS activators is needed. In this study, iron–nitrogen-carbon (Fe-N-C) activators were prepared using covalent organic frameworks containing homogeneous micropores and high porosity as a precursor. The Fe-N x -rich activator showed an outstanding activity and a high stability in the heterogeneously activated PMS system. It found that the 10 mg/L paracetamol (PCT) could be degraded completely within 5 min when adding 30 mg/L activator and 3 mM PMS. Furthermore, the system shows good performance in an extensive buffer pH range (2.6–10.67). The quenching experiments and intermediate product tests supported that the high-valent iron-oxo species is the major reactive oxygen species (ROS) in this system, and the designed experiments confirmed that Fe-N as the active site that in charge of activating PMS. This work provides insights for improving the activation efficiency and expanding the pH working range of iron-based catalysts in the field of advanced persulfate oxidation .
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 Water Process Engineering
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2024
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IF 6.3
S. Jafari,A.R. Faraji,A. Gil,F. Ashouri
Valorizing single-use plastic waste as an effective activator in environmental protection has gained great interest from policymakers, legislators, and scientific research communities. Herein, low-cost and highly porous alkali Fe/Mn-doped carbon nanomaterials derived from polyethylene terephthalate (PET) waste (MF/ c PET- x ) were fabricated via facile pyrolysis and alkali-metal impregnation methods. Detailed characterizations of MF- c PET- x demonstrated that the ratio of alkaline impregnation and pyrolysis temperature affects the porous characteristics, content, and size of active sites, specific surface area, and yield of carbon residue/nanocomposite. The main aim of this study was to evaluate and optimize the MF/ c PET- x applied for the detoxification of various kinds of pharmaceutical drugs ( tetracycline , naproxen , paracetamol , and levofloxacin ) and various dyestuff in their single, binary, ternary, and quaternary solutions. The magnetic porous MF/ c PET-1 was found to show a most effective PMS activation for single/multiple toxic pollutants removal attaining levels >91.0 % in a wide range of temperatures (5–35 °C) and pH (3.0–9.0), without significant detectable metal leaching (>0.16 mg L −1 ). The outstanding catalytic performance in complex water environments was mainly attributed to the deposition of Mn/Fe nanoparticles with small grain size on a polymeric scaffold, bimetal synergistic effect, high specific surface area, high stability, and excellent anti-interference capability against coexisting substances. Physicochemical properties of the recycled composite, masking, and EPR analyses confirmed that the dominant reactive species in the following order: 1 O 2 > OH > SO 4 − > O 2 − . This work offers a new and straightforward approach for preparing porous alloy composite from plastic waste for pollutant degradation in various water matrices.
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 Materials Chemistry A
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2024
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IF 10.7
Chao Yuan,Jialing Sheng,Shuke Guo,Xiaoyu Wang,Jiangyan Xu,Hongmei Jiang
In this work, a magnetic CoFe alloy and Co supported on mesoporous carbon with abundant defects (CoFe–Co/MC) was prepared by a sol–gel method combined with calcination and applied to activate peroxymonosulfate (PMS) and efficiently remove bensulfuron methyl (BSM) from water. CoFe–Co/MC could degrade 95% of BSM, while Co or Fe without supported mesoporous carbon could only provide degradation efficiencies below 10%, indicating that the introduction of mesoporous carbon could effectively enhance catalytic activity. Moreover, the dissolution of Co2+ from CoFe–Co/MC is only 0.22 mg L−1, which is about 20% of Co/MC, indicating that the bimetallic composite effectively inhibits the dissolution. The results of radical scavenger and EPR experiments demonstrated that 1O2 played the leading role in degradation process, while SO4˙− and small amounts of ˙OH and O2˙− were also involved in the degradation. The results of p-BQ scavenger and N2 atmosphere experiments showed that 1O2 mainly originated from the interaction between carbon defects and dissolved oxygen. The degradation performance of the CoFe–Co/MC/PMS system, carbon defect content and 1O2 content all increased with the increase of pyrolysis temperature, which demonstrated that adjusting pyrolysis temperature can regulate carbon defect content and 1O2 content, further improving catalytic activity. Possible BSM degradation pathways of CoFe–Co/MC/PMS were investigated in detail. This research provides new insights into the design and construction of metal–carbon catalysts rich in carbon defects and reveals how to regulate carbon defect content, 1O2 content and catalytic performance.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xinran Li,Jian Chen,Zaiyu Liu,Chengyu He,Jian Pang,Lilei Zhang,Fenglin Tang,Xiupei Yang
A bimetallic MOF derivative consisting of Fe and Co (Fe/Co 2 -MOF) by Co-doping MIL-101(Fe) was successfully synthesized for peroxymonosulfate (PMS) activation in acetaminophen (N-Acetyl-Para-Amino-Phenol, APAP) degradation. The presence of Co significantly accelerated the transfer of electrons due to the synergistic effect between Fe and Co bimetallic sites. Specifically, the reaction rate constant of APAP in the Fe/Co 2 -MOF + PMS system was three orders of magnitude higher than that of MIL-101(Fe) alone and 90 times higher than that of the MIL-101(Fe) + PMS system, respectively. At room temperature, 100 % of the APAP was degraded in 15 min with a Fe/Co 2 -MOF concentration of 0.05 g/L and a PMS concentration of 0.8 mmol/L across a wide pH range from 3 to 9. High-valence metal species (Co IV and Fe IV ) and electron transfer-dominated nonradical processes were responsible for the APAP degradation. Although singlet oxygen ( 1 O 2 ) was identified as the main active species in our study, the relative contribution of 1 O 2 was negligible. The catalytic performance was particularly notable in the practical implementation of hospital sewage treatment. However, it is still urgent to seek ways to relieve cobalt leaching of Fe/Co 2 -MOF. This strategy of Co-doping provides a clear illustration of modulating MIL-101(Fe) ultimately maximize their catalytic efficiency in PMS activation for water purification.
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高影响因子
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