JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Qi Yang,Dan Chen,Libing Chu,Jianlong Wang
In present work, we studied a novel Fe/C nanomaterial fabricated using Fe-based metal organic frameworks (MOFs) as precursors through thermal pyrolysis to catalyze gamma irradiation-induced degradation of antibiotics, cephalosporin C (CEP-C) and sulfamethazine (SMT) in aqueous solution. The MOFs-derived Fe/C nanomaterials (DMOFs) had the regular octahedrons structure of MOFs and contained element C, Fe and O, while Fe° with a fraction of Fe 3 O 4 and Fe 2 O 3 were identified. Results showed that DMOFs addition could accelerate the generation of OH during gamma irradiation, while the intermediates of bonds cleavages of antibiotic molecules and OH addition were identified. DMOFs were more effective to improve the decomposition of antibiotic having the higher adsorption capacity like SMT. The degradation rate of CEP-C and SMT increased by 1.3 times and 1.8 times, and TOC reduction at 1.0 kGy reached 42 % and 51 %, respectively by gamma/DMOFs treatment, while only 20.2 % (CEP-C) and 4.5 % (SMT) of TOC reduction were obtained by γ-irradiation alone. The crystal structure, functional groups and magnetism of DMOFs changed slightly after gamma irradiation, which made it possible to be reused. DMOFs were promising to enhance the degradation of antibiotics during gamma irradiation.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Haoyang Wu,Zhilong Tan,Bin Miao,Hailong Hu,Sanying Hou
In this work, Fe, N co-doped hierarchical porous graphite-like carbon with carbon-encapsulated Fe/Fe 3 C@ Fe-N-C was synthesized by a facile solid-phase synthesis strategy, and was employed as an efficient catalyst to activate peroxymonosulfate (PMS) for oxidation of tetracycline (TC). The optimal Fe-N/C 800 outlined a highly catalytic performance in activating peroxymonosulfate (PMS) with TC decomposition rate reaching 89.2 % in 20 min at ultra-low catalyst dosage. Meanwhile, the effect of operating parameters was also investigated in order to evaluate the potential of using Fe-N/C 800 in practical applications. In addition, the characterization analysis and experiments results elucidated that graphitic N, pyridinic N, C O, Fe 3 C, Fe 0 and FeN 4 were considered as the main reactive species promoting the PMS activation to generate reactive oxygen species (ROS) (including singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 •- ) and hydroxyl radical (•OH)). The electron paramagnetic resonance (EPR) experiments and radicals quenching analyses further demonstrated that the non-radical species singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species. Moreover, the TC degradation pathways were presented by LC-MS. Ultimately, the toxicity of the intermediate products were also investigated by ECOSAR system.
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CLAY MINERALS
·
2023
·
IF 1.5
Qinkai Lei,Yahui Lv,Chengshuai Liu,Wenpo Xu,Shujie Hu,Manjia Chen,Hongling Bu,Junhui Li
Mineral–organic matter (OM) associations play an important role in determining the long-term retention of OM in soils. However, the retention mechanisms of OM in cation–mineral–OM systems remain unclear. Taking into account the dominance of montmorillonite (Mnt) in the soil of the temperate zone, we investigated the stability of humic substances (HSs) in the Fe(III)–Mnt–HS system using thermal analysis. The HS degradation started at ~387°C in the Fe(III)–Mnt–HS system, which was higher than that of the Fe(III)–HS system (290°C). The formed ferrihydrite (Fhy) mainly contributed to the enhanced labile OM retention through adsorption and/or co-precipitation, whereas Mnt inhibited the initial formation and subsequent transformation of Fhy, thus improving the stability of OM. These results suggest that the HS stability in Fe(III)–clay–HS systems depends on the Fe speciation affected by clay minerals, and this finding provides insights into OM–mineral interactions in temperate-zone soils.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Junyuan Zhang,Ziwei Deng,Shuli Bai,Changyu Liu,Mengchen Zhang,Chao Peng,Xiaolong Xu,Jianbo Jia,Tiangang Luan
In this work, potassium acetate (KAc) was added during the synthesis of a Zn-Fe based metal-organic framework (Fe-ZIF-8) to increase the fixed amount of Fe while simultaneously enhancing the number of pores. Electrospinning was utilized to embed KAc-modified Fe-ZIF-8 (Fe-ZIF-8-Ac) into the polyacrylonitrile nanofiber mesh, to obtain a network composite (Fe@NC-Ac) with hierarchical porous structure. Fe@NC-Ac was co-pyrolyzed with thiourea , resulting in Fe, N, S co-doped carbon electrocatalyst . The electrochemical tests indicated that the prepared catalyst displayed relatively remarkable oxygen reduction reaction (ORR) catalytic activity, with an onset potential (E onset ) of 1.08 V (vs. reversible hydrogen electrode, RHE) and a half-wave potential (E 1/2 ) of 0.94 V, both higher than those of the commercial Pt/C (E onset = 0.95 V and E 1/2 = 0.84 V), respectively. Assembled into Zn-air batteries, the optimized catalyst exhibited higher open circuit voltage (1.698 V) and peak power density (90 mW cm −2 ) than those of the commercial 20 wt% Pt/C (1.402 V and 80 mW cm −2 ), respectively. This work provided a straightforward manufacturing strategy for the design of hierarchical porous carbon-based ORR catalysts with desirable performance.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Guang Li,Yiqiao Zhang,Xue Zhang,Jian Zhang,Bo Sun
This study delves into the formation of ferryl ions (Fe(IV)) within the Fe(II)/peroxydisulfate (PDS) process, a pivotal reaction in advanced oxidation processes (AOPs) aimed at organic pollutant removal. Our findings challenge the conventional view that Fe(IV) predominantly forms through oxygen transfer from PDS to Fe(II), revealing that sulfate radicals (SO4•–) play a crucial role in Fe(IV) generation. By employing competitive kinetics, the second-order rate constant for Fe(III) oxidation by SO4•– was quantified as 4.58 × 108 M–1 s–1. Factors such as the probe compound concentration, chloride presence, and iron species influence Fe(IV) generation, all of which were systematically evaluated. Additionally, the study explores Fe(IV) formation in various Fe(II)-activated AOPs, demonstrating that precursors like peroxymonosulfate and H2O2 can also directly oxidize Fe(II) to Fe(IV). Through experimental data, kinetic modeling, and oxygen-18 labeling experiments, this research offers a comprehensive understanding of the Fe(II)/PDS system, facilitating the optimization of AOPs for pollutant degradation. Finally, introducing HSO3– was proposed to shift the Fe(II)/PDS process from Fe(IV)-dominated to SO4•–-dominated mechanisms, thereby enhancing pollutant removal efficiencies.
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Chemical Science
·
2024
·
IF 7.6
Wei-Xing Chen,Zi-Sheng Li,Harry W. T. Morgan,Cong-Cong Shu,Zhong-Ming Sun,John E. McGrady
We report here the synthesis and characterization of two endohedral Zintl-ion clusters, [Fe4Sn18]4− and [Fe4Pb18]4−, which contain rhombic Fe4 cores. The Fe–Fe bond lengths are all below 2.5 Å, distinctly shorter than in the corresponding Cu clusters, indicating the presence of Fe–Fe bonding. Subtle differences in the structure of the Fe4 core between the two clusters suggest that the change in tetrel element causes a change in electronic ground state, with a very short Fe–Fe bond length of 2.328 Å present across the diagonal of the rhombus in the lead case.
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LANGMUIR
·
2024
·
IF 3.7
Zewen Fan,Wannan Wang,Jing Ren,Shaofei Zhang,Ruipeng Ren,Yong-Kang Lv
Fe[Fe(CN)6] (FeHCF) is considered a promising material for capacitive deionization–desalination of saline wastewater due to its excellent structure. However, additives are usually introduced during the synthesis of FeHCF in order to avoid [Fe(CN)6]3– vacancy defects filled by ligand water, which can result in the appearance of harmful byproducts and additional water treatment costs. In this study, an additive-free in situ vacancy repair strategy is proposed for the rapid synthesis of high-quality FeHCF in a saturated K3Fe(CN)6 solution. During the process of synthesizing FeHCF in solution, a high concentration of [Fe(CN)6]3– is found to facilitate the binding of Fe3+ to [Fe(CN)6]3– and hinder the hydrolysis and coordination reaction of Fe3+. After undergoing repair, FeHCF4 demonstrates an increased capacity and highly reversible electrochemical performance due to the robust structure. When utilized as Faraday cathodes in hybrid capacitive deionization (HCDI) systems, FeHCF4 exhibits a higher salt removal capacity (65.67 mg g–1) and lower energy consumption (0.68 kWh kg–1-NaCl) compared to unrepaired FeHCF1, while still maintaining excellent cycling performance. This environmentally friendly approach of repairing vacancies serves as a source of inspiration for the advancement of high-performance Prussian Blue analogues as capacitive sodium-removing materials.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Yunpeng Zha,Xiaoxiao Sun,Zhengjun Xiong,Dandan Dong,Shili Li,Qinqin Wang,Minmin Liu
The porous carbon materials co-coordinated with Fe and N (Fe-N-C) were successfully synthesized through one-step pyrolysis with the zeolitic imidazolate framework (ZIF-8) as the precursor. Through systematic optimization of iron ion concentration during synthesis, the Fe-N-C-20 specimen exhibited optimal adsorption performance toward dibenzothiophene (DBT), demonstrating a maximum sulfur adsorption capacity of 22.14 mg S/g with a corresponding removal efficiency of 92 %. This superior performance can be primarily ascribed to the formation of Fe-S bonds anchored on Fe-N active sites, N-S interactions mediated by graphitic nitrogen species and appropriate pore size that allows access to thiophenic compounds. Furthermore, the experimental adsorption isotherms for DBT exhibited strong correlation with the Density Functional Theory (DFT) calculation. Additionally, the material's adsorption process followed pseudo-second-order kinetics and Langmuir isotherms of Fe-N-C, and the pseudo-second-order model shows the smallest RMSE (0.66), extremely low SSE (3.03) and AIC (-1.86), which further proves its excellent fitting ability. And the best balance between parameter efficiency and fitting performance. The high stability and recyclability of ZIF-derived Fe-N-C porous adsorbents contribute to sustainable industrial practices.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haonan Chen,Shiqi Tian,Zheng-Qian Liu,Jun Ma,Gang Wen
Iron oxides are widely utilized in catalytic ozonation, but their effectiveness is often limited by the slow Fe(II)/Fe(III) redox cycle. In this study, a series of metal sulfide–iron oxide composites were synthesized, all of which exhibited enhanced catalytic performance, with MoS 2 @Fe 3 O 4 showing outstanding efficiency. The catalytic system decomposes ozone (O 3 ) into hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ), with ·OH predominantly contributing to the oxidation process. The catalytic process was significantly enhanced through three key pathways: (i) metal sulfides themselves demonstrate superior ozonation catalytic performance compared to iron oxides; (ii) the presence of Mo(IV) effectively promotes the Fe(II)/Fe(III) redox cycle; and (iii) the transient superoxide radical (·O 2 − ), a crucial intermediate in ozone chain decomposition, rapidly reduces high-valence Mo(VI) to Mo(IV), thereby reinforcing the Mo redox cycle, further strengthening the Fe redox cycle, and leading to the accumulation of 1 O 2 . Notably, the efficient utilization of ·O 2 − represents a unique mechanism in the catalytic ozonation system. These findings emphasize the critical role of the Mo redox cycle in enhancing Fe redox activity to promote catalytic ozonation, providing valuable insights for the development of advanced metal sulfide–iron oxide catalysts for environmental applications.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 35
·期 8
·e6280
·
IF 4.105
Jinzhong Guo,Zhuming Guo,Zhiyin Xiao,Jing Jin,Xiuqin Yang,Yi He,Xiaoming Liu
Four new monoiron (II) tricarbonyl complexes with the amine bound, fac -[Fe(CO) 3 I 2 (NH 2 R)] (R = Et, 1 ; n Pr, 2 ; n Bu, 3 ; n Pent, 4 ), were reported using cis -[Fe(CO) 4 I 2 ] as the precursor. All the complexes 1 – 4 were structurally confirmed by various techniques such as ultraviolet–visible (UV–vis), Fourier transform infrared (FTIR), and nuclear magnetic resonance (NMR) spectra and elemental analysis of which complexes 1 and 2 are crystallographically determined. The reaction of the precursor with alkylamines proceeded in two main parallel pathways to form both aminium salts of fac -[Fe(CO) 3 I 3 ] − and the amine-bound complexes ( 1 – 4 ). Their dominances altered with the reaction time. These complexes in DMSO undergo quick decomposition with complex 1 as the relatively most stable one ( t 1/2 = 7.3 min) although they are stable in solid status. Unlike the triiodo anion and pyridinyl analogs showing severe cytotoxicity due to the generation of iodine radical during the decomposition, no iodine radicals were detected from the fac -[Fe(CO) 3 I 2 (NH 2 R)] complexes. Therefore, the cell viability of RT112 cells was not affected by the presence of the amine-bound iron complex ( 1 ) up to 100 μmol L −1 .
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Feng Cheng,Peng Zhou,Yang Liu,Xiaowei Huo,Jian Zhang,Yue Yuan,Heng Zhang,Bo Lai,Yongli Zhang
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of H 2 O 2 to produce hydroxyl radicals ( • OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/H 2 O 2 Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that • OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote H 2 O 2 induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/H 2 O 2 systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/H 2 O 2 system with or without visible light shows high potential for application in environmental remediation.
研究领域:
环境科学
·
化学
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Chemical Engineering Journal Advances
·
2021
·
IF 0
Kai Wei,Xiufan Liu,Shiyu Cao,Huijuan Cui,Yu Zhang,Zhihui Ai
In this study, we fabricated a micro-nano structured Fe 2 O 3 @FeB composites by treating commercial Fe 2 O 3 with sodium borohydride. The outside amorphous FeB alloy shell endowed the Fe 2 O 3 @FeB with remarkable Fenton-like performance in organic pollutants oxidation by efficient Fe(III)/Fe(II) cycle. For instance, the pseudo first-order rate constants of RhB degradation using Fe 2 O 3 @FeB as Fenton reagent was 74.6 times that of the Fe 2 O 3 counterpart, the hydroxyl radical generation rate of Fe 2 O 3 @FeB was 1-3 orders of magnitude larger than that of other heterogeneous Fenton reagent. Further mechanistic study unveiled that FeB was oxidized accompanying with Fe(0) and B(0) continuously donated electrons to Fe(III) to secure the efficient generation of surface Fe(II), which could generate additional H 2 O 2 by consecutive single-electron molecular oxygen activation (O 2 →•O 2 − →H 2 O 2 ), leading to enhance •OH production and Fenton-degradation toward typical pollutants. This study provides a facile route for efficient heterogeneous Fenton and strengthens the vital role of molecular oxygen activation on Fenton-like process.
研究领域:
环境科学
·
材料科学
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