LANGMUIR
·
2024
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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.
研究领域:
材料科学
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环境工程
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Junhui Yang,Wenlei Wang,Jinglin Yin,Yanmei Li,Ziyang Xiang,Yi Peng,Ying Yan,Jing Wang,Hongbo Xiao
In this study, a matrix composite material of CdZnS and α-FeOOH on carbon cloth (CZS@FeOOH@CC) was prepared by a hydrothermal method , and was used for the degradation of As(III). The composite material has good photocatalytic activity of removing As(III) in the presence of oxalate. CZS@FeOOH@CC can completely degrade 10 mg/L As(III) within 10 min under visible light irradiation. The influence factors of CZS@FeOOH@CC composite material on catalytic oxidation of As(III) were also studied in the oxalate system. The photocatalytic oxidation efficiency of As(III) is affected by the oxalate concentration in the reaction system, and the atmosphere plays a major role in the degradation of As(III). Under visible light, oxalate first combines with Fe(III) on the surface of iron oxide to form Fe(III)-oxalate complex, and then the Fe(III)-oxalate composite is activated to produce·C 2 O 4 − . In the presence of oxygen, Fe(II) readily reacts with O 2 and oxidizes to Fe(III). The introduction of CdZnS promoted the separation of interfacial electron holes, and accelerated the REDOX cycle of Fe(II)/Fe(III). This study provides a feasible and simple method for accelerating the catalytic removal of heavy metals from wastewater by iron-based materials.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
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2023
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IF 4
Zhang Xue-Feng,Chang Tian-Long,Guo Na,Jia Guo-Liang,Li Xiao-Bing,Zhao Zhao-Ye,Wang Hui,Wang Jun-Chuan,Wu Xiang-Feng,Pan Cheng-Si,Liu Lei,Yang Lin-Lin
Fe-based MOFs (Fe-MOFs) are excellent photocatalysts and have synergy well with Fenton reagents relative to other MOFs. In this work, a series of uniformly covered NH 2 -Fe-MIL-88B@TpPa-1-COF composites were synthesized using an in-situ anchoring growth strategy, which used F127 as functional molecule to decorate NH 2 -Fe-MIL-88B nanoparticles to eliminate their surface electrostatic repulsion with Tp molecules during the subsequent coating procedure. Meanwhile, the -NH 2 groups in the skeleton of NH 2 -Fe-MIL-88B could also be used as anchors to covalently connect TpPa-1-COF shell and migration channels for effective charge transfer. This uniformly covered core–shell structure would endow these composites with much more contact area and imine bond linkage between the Fe-MOFs core and COFs shell. Compared with the random packing structure, the uniformly covered Fe-MOF@COF-3 composite possessed a higher proportion of Fe 2+ to Fe 3+ . As a result, the optimized Fe-MOF@COF-3 catalyst could achieve the highest photo-Fenton degradation efficiency of 93.9% for tetracycline hydrochloride (TC⋅HCl), which was much higher than 54.8% of pure NH 2 -Fe-MIL-88B. In addition, the uniform TpPa-1-COF shell could further effectively enhance the stability of NH 2 -Fe-MIL-88B by protecting Fe ions from leaching, and the toxicity of the water samples treated with our photo-Fenton degradation process declined obviously. All these merits will endow Fe-MOF@COF-3 photo-Fenton catalyst great potential application value as in the field of environmental governance.
研究领域:
材料科学
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环境科学
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催化
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yanjing Wang,Minglei Song,Jianrong Wei,Jie You,Siping Chen,Shuangyin Wang,Yanyong Wang
Electrochemically mediated Fe(II)/Fe(III) redox-coupled uranium extraction can efficiently reduce the cell voltage of electrochemical uranium extraction (EUE). How to regulate the surface structure to enhance the uranium acyl ion adsorption capacity and strengthen the Fe(II)/Fe(III) redox cycle process is crucial for EUE. In this work, we developed surface sulfated nanoreduced iron (S-NRI) for EUE and exhibited improved properties for EUE at an ultralow cell voltage (−0.1 V). Compared with a nanoreduced iron (NRI) adsorbent, S-NRI displayed faster electrochemical extraction kinetics properties and higher extraction efficiency and capacity for uranium. In a more complex seawater electrolyte containing uranyl ion concentration ranging from 1 to 20 ppm, the removal efficiency could reach almost ∼100% after EUE for 24 h. At a higher 50 ppm uranium acyl ion concentration in a seawater electrolyte, S-NRI exhibited higher extraction capacity (755.03 mg/g), which is better than 528.53 mg/g of NRI at a cell voltage of −0.1 V. Outstanding EUE property could be attributed to the fact that sulfate species (M–SO42–) on the S-NRI surface not only enhanced selective adsorption of uranyl ions but also strengthened the Fe(II)/Fe(III) redox cycle, which accelerated electron transfer between Fe(II) and U(VI), promoted the regeneration of Fe(II) active sites, and finally enhanced the EUE property.
研究领域:
材料科学
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环境科学
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电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Jie Zhang,Xufei Wang,Yiwei Liu,Tao Jin,Liang Liu,Xiaodong Ma,Gengbo Ren
The efficiency and stability of the electrical activation of persulfate (PS) by transition metal-based cathode are controlled by the cycling of Fe(III)/Fe(II) and the mass transfer of PS. In this study, the mixed-valence MOFs catalyst (Fe II -MIL-53(Fe)) modified flow-through cathode was prepared for the first time. Fe II -MIL-53(Fe) was prepared by replacing part of the iron-oxygen network structure in MIL-53(Fe) with Fe(II), resulting in the formation of coordinated unsaturated iron centers (CUICs). The increase of the Fe(III) CUICs facilitated the conversion of Fe(III) to Fe(II). Furthermore, the cycling of Fe(III)/Fe(II) was further promoted by the electric field. Meanwhile, the hydrodynamic behavior of flow-through cathode was indicated by the computational fluid dynamics (CFD) simulation. The quenching experiments and electron paramagnetic resonance (EPR) results showed that several reactive specie (SO 4 ·- , ·OH, O 2 ·- and 1 O 2 ) were produce. In summary, this work provided an effective strategy for the efficient and stable electrical activation of PDS.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Yanan Wei,Bingfeng Wang,Xinfang Cui,Yaseen Muhammad,Yanjuan Zhang,Zuqiang Huang,Xuesheng Li,Zhenxia Zhao,Zhongxing Zhao
MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp2 C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer–Emmett–Teller: 1730 m2/g). Liquid chromatography–mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe–N, −587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)/Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 °C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77851-77863
·
IF 5.19
Jiang Changjin,Zhang Ting,Li Shuhui,Yang Zhaoguang
Fe(III)-chitosan and Fe(III)-chitosan-CTAB composites were prepared using an ionotropic gelation method. Various techniques were used to analyze the morphology, structure, and property of the adsorbents, including SEM, EDS, FT-IR, XPS, and zeta potential. Compared with Fe(III)-chitosan, Fe(III)-chitosan-CTAB was more effective for As(V) adsorption at a wide range of pH (3.0–8.0). The adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB could reach equilibrium in 20 min, and their maximum adsorption capacities were 33.85 and 31.69 mg g ‒1 , respectively. The adsorption kinetics was best described by the pseudo-second-order model ( R 2 = 0.998 and 0.992), whereas the adsorption isotherm was fitted well by the Freundlich model ( R 2 = 0.963 and 0.987). The presence of H 2 PO 4 – significantly inhibited the adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB, and humic acid also led to a slight decrease in As(V) adsorption by Fe(III)-chitosan-CTAB. Over 94% of As(V) at the initial concentration of no more than 5 mg L –1 was removed from real water by the two adsorbents. 1% (w/v) NaOH solution was determined to be the most suitable desorption agent. Fe(III)-chitosan and Fe(III)-chitosan-CTAB still maintained their initial adsorption capacities after five adsorption–desorption cycles. Based on different characterization results, both electrostatic attraction and surface complexation mechanisms played important roles in As(V) adsorption on Fe(III)-chitosan and Fe(III)-chitosan-CTAB.
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
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jialong Yin,Heng Zhang,Mengfan Luo,Jia Zhao,Bingkun Huang,Pinji Chen,Zhenpeng Cai,Yue Yuan,Yang Liu,Chuanshu He,Bo Lai
The ferrous species (Fe(II))-periodate (PI) system employs efficient decontamination by generating ferryl species (Fe(IV)-oxo) under acidic pH conditions. However, the mechanisms by which the Fe(II)/PI system operates across a broad pH range remain elusive. In light of the rapid oxidation and consumption of Fe(II) at neutral pH, we developed an electro-Fe(II) system utilizing an iron plate anode to activate PI (E(Fe/C)/PI). Efficient sulfamethoxazole (SMX) degradation was achieved under the E(Fe/C)/PI system across a range of pH values. Quenching and chemical probe experiments revealed a transition from Fe(IV)-oxo to singlet oxygen ( 1 O 2 ) as the predominant reactive species from acidic to near-neutral pH, respectively. Density functional theory (DFT) calculations indicated that the differences in one-electron transfer capacity and hydrolysis pathways for various protonated Fe(IV)-oxo species underlie the variations in catalytic mechanisms. This study not only enhances the efficiency of the Fe(II)/PI system but also provides a comprehensive understanding of the activation mechanisms at different pH levels.
研究领域:
环境化学
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电化学
·
催化
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiangshun Wu,Hanpei Yang,Li Kang,Zhao Gao,Feifan Ren
In this work, a series of Fe-based metal-organic frameworks (Fe-MOFs) were synthesized and served as Fenton-like catalysts for tetracycline hydrochloride (TC–HCl) degradation. Herein, for the first time, we have demonstrated that visible light can accelerate Fe(II)/Fe(III) cycle in the photo-Fenton system based on iron-oxo (Fe-O) clusters in frameworks. Among these Fe-MOFs, MIL-101 possessed the highest activity mainly ascribed to its largest specific surface area and pore volume, and the most coordinatively unsaturated iron sites. The synergistic effect in the MIL-101/H 2 O 2 /visible light system was derived from the efficient separation and migration of photogenerated carriers. Due to the function of solid acid catalysts, MIL-101 extended effective pH range up to 10.2 and exhibited good reusability and stability. Hydroxyl radicals generated from H 2 O 2 coordinated at iron active sites were determined as the main reactive oxidative species and acceleration of Fe(II)/Fe(III) cycle was responsible for highly effective degradation of TC–HCl.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2020
·
IF 3.408
Yanan Dong,Tianding Hu,Manoj Pudukudy,Hongying Su,Lihong Jiang,Shaoyun Shan,Qingming Jia
In this paper, the effect of conventional solvothermal and a microwave-assisted method for the synthesis of MIL-101(Fe) and NH 2 -MIL-101(Fe) as adsorbents for the removal of tetracycline in wastewater is reported for the first time. The results had shown that the microwave treatment led to a significant reduction in the material synthesis time, which greatly saved the energy. It was also found that the microwave-assisted synthesized material exhibited small particle size, high specific surface area and better adsorption capacity. The introduction of amino group further enhanced the adsorption capacity of MIL-101(Fe). The adsorption capacity of MIL-101(Fe) and NH 2 -MIL-101(Fe) samples for tetracycline adsorption by microwave assisted synthesis method reached up to 332 mg/g and 378 mg/g, respectively. Moreover, the adsorption isotherm was well-fit with Freundlich model, indicating a multilayer adsorption . The kinetic studies indicated that the reaction followed pseudo second-order reaction kinetics with a best fit to the theoretical value. Due to the higher adsorption efficiency and lower energy consumption of the synthesis, the as-prepared microwave assisted materials could be used as potential adsorbents for different pollutants in wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）