ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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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
·
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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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 46
·19700-19707
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IF 2.7
Nan Zhou,Fanyi Kong,Ya Tang
The traditional impregnation method for preparing supported catalysts often faces challenges such as particle agglomeration and weak support–metal interactions. This study focuses on utilizing the exsolution method to prepare Fe, Co, and Ni supported catalysts from ABO3-type perovskites, aiming to overcome these challenges. Experimental results show that LaBO3 perovskites with different B site metals (B = Fe, Co, Ni) exhibit different metal exsolution kinetics in the ammonia synthesis reaction. LaNiO3 demonstrates an initial activity of 782.2 μmol g−1 h−1 within the first 2 hours of the reaction, maintaining stability beyond 80 hours. In contrast, LaFeO3 and LaCoO3 exhibit prolonged initiation periods for the metal exsolution process, reaching activities of 7873.8 μmol g−1 h−1 and 8046.7 μmol g−1 h−1, respectively, after approximately 80 hours. The degree of B-site metal exsolution was investigated using X-ray absorption fine structure (XAFS) and Rietveld refinement of XRD data, revealing exsolution rates of 72.03%, 69.3%, and 86.3% for Fe, Co, and Ni, respectively, after 80 hours of reaction. This study not only introduces the exsolution method for ammonia synthesis but also empirically validates several computational predictions, thereby supporting both theoretical and practical research.
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Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 21
·3213-3224
·
IF 8.683
Wenfang Miao,Feirong Huang,Xiaochen Shen,Shaopeng Li,Xingru Cao,Xuefeng Zhang,Jieyi Yu,Xinglong Dong
The development of high-efficiency, stable, and low-cost Fe–N–C electrocatalysts for the oxygen reduction reaction (ORR) has attracted considerable attention. Herein, a stable atomically dispersed Fe–Nx-based catalyst was synthesized from a hierarchical structure involving carbon nanofiber (CNF)-supported zeolitic-imidazolate-framework-8 (ZIF-8) encapsulated Fe–Phen complex ((Fe,N)-ZIF-8/CNFs). The Fe–Nx–CNFs obtained from the pyrolysis of (Fe,N)-ZIF-8/CNFs showed a good hierarchical multi-layer structure. The natural network structure of the carbon nanofibers serves as a matrix to uniformly distribute the ZIF-8 particles, and the Fe–Nx sites derived from the Fe–Phen complex were uniformly distributed in ZIF-8 particles. It exhibits excellent ORR performance with a high half-wave potential of 0.875 V (vs. RHE), which was 55 mV higher than that of the commercial Pt/C catalyst. In addition, density functional theory (DFT) calculations on the catalyst further revealed the origin of the ORR activity via a 4e− pathway from the precise local coordination of FeN4 sites.
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iScience
·
2021
·
IF 5.458
Yanfei Zeng,Xinyi Zhang,Xianxing Mao,Pei Kang Shen,Douglas R MacFarlane
The Ni-Fe battery is a promising alternative to lithium ion batteries due to its long life, high reliability, and eco-friendly characteristics. However, passivation and self-discharge of the iron anode are the two main issues. Here, we demonstrate that controlling the valence state of the iron and coupling with carbon can solve these problems. We develop a mesostructured carbon/Fe/FeO/Fe 3 O 4 hybrid by a one-step solid-state reaction. Experimental evidence reveals that the optimized system with three valence states of iron facilitates the redox kinetics, while the carbon layers can effectively enhance the charge transfer and suppress self-discharge. The hybrid anode exhibits high specific capacity of 604 mAh⋅g -1 at 1 A⋅g -1 and high cyclic stability. A Ni-Fe button battery is fabricated using the hybrid anode exhibits specific device energy of 127 Wh⋅kg -1 at a power density of 0.58 kW⋅kg -1 and maintains good capacity retention (90%) and coulombic efficiency (98.5%).
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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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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Rong Chen,Hui Liu,Man Tong,Lei Zhao,Peng Zhang,Deng Liu,Songhu Yuan
The interplay of Fe(II) oxidation and Fe(III) bio-reduction occurs widely in both natural and engineered redox-dynamic systems. This study aimed to unravel the impact of Fe(II) oxidation by O 2 in the presence of iron-reducing bacteria on subsequent Fe(III) bio-reduction. Mixed solutions of Fe 2+ (0.1–0.5 mM) and Shewanella oneidensis strain MR-1 (MR-1, 2.0 × 10 7 CFU/mL) at neutral pH were first exposed to laboratory air for Fe(II) oxidation and bacterial inactivation, and then the resultant Fe(III) suspensions were switched to anoxic conditions for bio-reduction by the surviving bacteria. In the oxidation step, the coexisting MR-1 was inactivated by 0.8–1.71 orders of magnitude within 60 min. In the subsequent bio-reduction step, the resultant Fe(III) was bio-reduced by the surviving MR-1. Bio-reduction of the resultant Fe(III) by the surviving MR-1 was 1.8–2.5 times faster than that of the Fe(III) that was produced from Fe 2+ oxidation without MR-1 by fresh MR-1 cells at 2.0 × 10 7 CFU/mL. Although MR-1 inactivation during Fe(II) oxidation may inhibit Fe(III) bio-reduction, the increase in bio-availability of the resultant Fe(III) and the residual reactivity of dead cells led to net enhancement of bio-reduction under the tested conditions. Lepidocrocite was the sole Fe(III) mineral that was produced from Fe 2+ oxidation without MR-1, while 19% ferrihydrite was produced from Fe 2+ oxidation in the presence of MR-1. The formation of low-crystallinity ferrihydrite accounts for the increase in bio-availability of the Fe(III) minerals. The findings of this study highlight an important but overlooked impact underlying the interplay of Fe(II) oxidation and Fe(III) bio-reduction.
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ChemElectroChem
·
2021
·Vol. 8
·期 24
·4817-4825
·
IF 4.59
Jie Zhu,Qian Zhang,Sudong Yang,Lin Chen,Peng Zhao,Qiang Yan
Graphical Flexibility approach : A facile two-step process for fabricating a distinctive Fe/Fe 3 O 4 composite deposited on carbon fabric as a negative electrode for a flexible nickel-iron battery is reported. The assembled battery exhibited a high voluminal capacity with a stable operating voltage up to 1.7 V, long-term cyclic stability as well as good mechanical stability and flexibility. The nickel-iron (Ni−Fe) battery is a competitive alternative for electrochemical energy storage, owning to its low cost, high safety, and strong auto-adaptive ability. However, the self-discharge and passivation of the negative electrode are the two main issues. In this work, a rock-like Fe/Fe 3 O 4 composite is synthesized and deposited on carbon fabric (Fe/Fe 3 O 4 @CF) by facile electrodeposition and annealing technologies to serve as a binder-free anode, which exhibits a large areal capacity of 0.466 mAh cm −2 and long-term cycling durability. Moreover, the flexible device is assembled by employing Fe/Fe 3 O 4 @CF-750 as anode and Ni(OH) 2 @CF as cathode. The above battery displays an enhanced operating voltage up to 1.7 V, impressive mechanical flexibility, outstanding cycling stability (86.2 % retention of initial value over 6000 charge-discharge cycles), and satisfactory voluminal capacity of 1.33 mAh cm −3 , indicating its potential application for energy supply systems of modern wearable electronics.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Heng Zhang,Mengfan Luo,Peng Zhou,Yang Liu,Ye Du,Chuanshu He,Gang Yao,Bo Lai
Recently, the enhancing role of hydrogen peroxide (H 2 O 2 ), a self-decay product of ferrate (Fe(VI)), on Fe(VI) reactivity has received increasing attention. In this study, we found that calcium peroxide (CaO 2 ) as a slow-releasing reagent of H 2 O 2 could also enhance the Fe(VI) performance for removing sulfamethoxazole (SMX). Compared with sole Fe(VI), sole CaO 2 and Fe(VI)-H 2 O 2 systems, the Fe(VI)-CaO 2 system showed higher reactivity to remove SMX. The radical scavenger and chemical probe test results indicated that the better oxidation performance of Fe(VI)-CaO 2 system than Fe(VI) alone was ascribed to the generation of Fe(Ⅳ) and Fe(Ⅴ) rather than • OH. In addition, the performance of Fe(VI)-CaO 2 system for degradation of contaminants was also superior to Fe(VI)-Na 2 SO 3 , Fe(VI)-NaHSO 3 and Fe(VI)-Na 2 S 2 O 3 systems under the same experimental conditions. Moreover, the effects of critical operating parameters, inorganic anions, inorganic cations, and humic acid on the degradation of SMX by Fe(VI)-CaO 2 system were revealed. The Fe(VI)-CaO 2 system exhibited good applicability in authentic water. Finally, the underlying degradation intermediates of SMX by Fe(VI)-CaO 2 system and their toxicity were confirmed. In conclusion, this study provides a new strategy for enhancing the oxidation capacity of Fe(VI) and comprehensively reveals the oxidation mechanism.
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FUEL
·
2021
·
IF 6.609
Xinyue Zhang,Bo Zhang,Yanjun Chen,Lei Li,Houxiang Sun,Xuandong Liu,Rong Guo,Bo Meng,Peng Liu,Weiyu Song,Qiaoxia Guo,Baojian Shen
Electronic structure tuning is an effective strategy to activate transition metals. In this study, silica-promoted γ-Al 2 O 3 -supported Fe-based hydrodesulfurization catalysts of Fe species with electron loss were successfully prepared by transferring electrons from Fe to Si. The characterization results showed that the Fe-based hydrodesulfurization catalyst with the addition of silica modulated the structure and properties of the active metal, which not only improved the degree of sulfidation of the active metal but also promoted the generation of Fe(III)-S. The hydrodesulfurization rate of dibenzothiophene showed a remarkable rise from 38.4 to 83.2% at 673 K. Importantly, the formation of Fe(III)-S greatly stretched the bond length of Fe-S bonds, exhibiting an increase of approximately 21%, this facilitating the generation of coordinatively unsaturated active site. Finally, the HDS reaction performance of the Fe-based hydrodesulfurization catalysts was mainly influenced by the Fe(III)-S/Fe(II)-S ratio, with the most significant enhancement in the direct desulfurization reaction path. The results of this study provide a promising approach for the design and development of environmentally friendly and economical Fe-based catalysts in the field of clean fuels.
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