MICROPOROUS AND MESOPOROUS MATERIALS
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2023
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IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Jin Huang,Jie Cao,Ni Tu,Huaping Dong,Jianfa Li,Jianxin Shou,Yimin Li
Nonionic and anionic surfactants often occur in anaerobic environments, but their roles in the removal of organic contaminants by Fe-bearing mineral/Fe(II) have not been determined. In this study, batch experiments were performed to investigate the effects of a nonionic surfactant (TX-100) and an anionic surfactant (SDBS) on the removal of nitrobenzene (NB) by Fe-bearing montmorillonite (FM)/Fe(II). Mössbauer spectrum and XPS were applied to analyze the edge surface bound Fe(II) and secondary minerals formed on FM. The contribution of surfactant to the enrichment of NB on FM was studied. The results showed that TX-100 and SDBS had opposite effects on the removal of NB by FM/Fe(II) at neutral pH. The presence of TX-100 improved the removal efficiency of NB from 36.4% to 70.0%, and increased the initial removal rate by 1.7 times. This enhancement effect was mainly attributed to the formation of more active edge surface bound Fe(II) that can reduce more NB to aniline. Formation of more magnetite on FM and selective enrichment of NB on the reactive surface also contributed to the removal of NB. In contrast, the presence of SDBS reduced the amount of edge surface bound Fe(II) via formation of SDBS-Fe(II) complex, which decreased the removal efficiency of NB.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
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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.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Hao Xu,Qian Ye,Jing Zhang,Qiansong Li,Meijing Wang,Peng Zhou,Guanyu Zhou,Qingguo Wang
In response to the inherent restriction of low Fe(II) regeneration in the Fenton process, this study demonstrated a mutual-promoting configuration, where oxygen functionalized g-C 3 N 4 (OCN) was applied in Fe(III)/H 2 O 2 system to utilize mild natural solar light (SL) for persistent Fe(II) generation. The constructed OCN/Fe(III)/H 2 O 2 /SL system exhibited strong adaptability to various pollutants, and it well outperformed the g-C 3 N 4 (GCN) modified system and the traditional Fenton system in pollutants degradation efficiency. Compared with GCN, OCN could significantly promote the Fe(II) generation under solar light (SL), leading to more efficient H 2 O 2 activation. The characterization analyses revealed the larger surface area and enhanced charge separation of OCN, which were considered to take main responsibility for its enhanced photoactivity. The complexation of Fe(III) with the carboxyl groups of OCN also benefited the Fe(II) generation. ·OH was detected as the dominant radical responsible for metronidazole (MNZ) degradation, and its production in the OCN modified system was about twice that in the GCN modified system and the Fenton system. Moreover, the precipitation of FeO x on the OCN surface benefited the charge separation of the OCN, so that the improved OCN enabled a slight enhancement of MNZ degradation in the reuse experiments. The intermediates of MNZ degradation were analyzed based on the results of LC-MS, which provided insight into MNZ degradation pathways. This work highlighted the concept of self-improving photocatalyst, the ingenious combination of photocatalysis and Fenton-like system formed a mutual-promoting situation where the OCN and the Fenton-like system could both be improved, which endowed the configuration great potential for green and economical oxidation in environmental remediation.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2026
·
IF 9.2
Lu Zeng,Xuexia Guo,Jiahao Sun,Wenbin Huang,Huinan Zhao,Lingling Hu,Shuanghong Tian,Chun He
In Fenton-like processes, achieving rapid and efficient redox cycling of metal active centers remains a challenge. This study presents an innovative strategy that harnesses the mechanical energy of water flow to drive the redox cycling of metal active centers. Herein, Fe 3 O 4 /MoS 2 heterojunction with interfacial Mo-S-Fe bridge bonds was constructed via a one-step hydrothermal method. Under the stimulation induced by water-flow mechanical, the piezoelectric effect of MoS 2 generates charge carriers, which are rapidly directed to Fe active sites through the Mo-S-Fe bonds. This process significantly accelerates the Fe(III)/Fe(II) cycle and enhances H 2 O 2 activation, achieving 93.8% removal of sulfamethoxazole (SMX) within 60 min under water flow stimulation. The composite exhibits robust performance across a broad pH range (3.0-10.7) and in the presence of humic acid (HA) and coexisting anions, demonstrating its strong environmental adaptability. Spectroscopic evidence confirmed the formation of Mo-S-Fe bonds at the heterojunction interface. Mechanistic studies further revealed that the structure improves charge separation, promotes rapid electron transfer from MoS 2 to Fe sites, and strengthens H 2 O 2 adsorption, thereby synergistically boosting reactive oxygen species (ROSs) generation and the overall catalytic efficiency. This study proposes an innovative strategy that exploits mechanical forces generated by water flow to drive rapid redox cycling of active metal centers in Fenton-like reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang
The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.
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iScience
·
2022
·
IF 6.107
Zheng Qian,Lingzhen Wang,Mawuli Dzakpasu,Yujia Tian,Dahu Ding,Rongzhi Chen,Gen Wang,Shengjiong Yang
The mechanism of spontaneous Fe III /Fe II redox cycling in iron-centered single-atom catalysts (I-SACs) is often overlooked. Consequently, pathways for continuous SO 4 ·- /HO⋅ generation during peroxymonosulfate (PMS) activation by I-SACs remain unclear. Herein, the evolution of the iron center and ligand in I-SACs was comprehensively investigated. I-SACs could be considered as a coordination complex created by iron and a heteroatom N-doped carbonaceous ligand. The ligand-field theory could well explain the electronic behavior of the complex, whereby electrons delocalized by the conjugation effect of the ligand were confirmed to be responsible for the Fe III /Fe II redox cycle. The possible pyridinic ligand in I-SACs was demonstrably weaker than the pyrrolic ligand in Fe III reduction due to its shielding effect on delocalized π orbitals by local lone-pair electrons. The results of this study significantly advance our understanding of the mechanism of spontaneous Fe III /Fe II redox cycling and radical generation pathways in the I-SACs/PMS process.
研究领域:
催化
·
环境化学
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材料科学
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Wenlong Zhang,Huanxin Li,Xiaohui Ning
The Fe/FeCl2-Graphite molten salt battery is a promising technology for large-scale energy storage, offering a long lifespan, a low operating temperature (<200 °C), and cost efficiency. However, its practical applications are hindered by the lack of a scalable preparation approach and insufficient redox stability in the Fe/FeCl2 electrode. Our study introduces an electrochemical anodic electrolysis (EAE) strategy, employing the anodic process (Fe → Fe2+) in an Al|AlCl3/NaCl/LiCl|Fe electrolysis system for the Fe/Fe2+ negative electrode in the Fe/FeCl2-Graphite battery. The EAE strategy forms an oxidized film, preventing incipient dissolution in the electrolyte and addressing redox stability issues with FeCl2 as the active substance. The Fe/Fe2+ negative electrode prepared by the EAE strategy exhibits a stabilized capacity of 0.72 mAh/cm2 after 7000 cycles at 5 mA/cm2, with a lower polarization level (∼29 mV) compared to FeCl2 as the active component. The flexibility of the EAE strategy is validated in both galvanostatic and potentiostatic processes, with a discharge capacity of 14 mAh after 1000 cycles, a capacity retention rate of 85%, and a Coulombic efficiency of 98% in the potentiostatic anodic electrolysis Fe/Fe2+ electrode. The scalability and reliability of the EAE strategy are further demonstrated in capacity-expanded Fe/FeCl2-Graphite batteries, reaching a discharge capacity of 155.1 mAh after 1000 cycles at 130 mA, with a capacity retention rate of 94%. For the first time, we showcased an EAE approach capable of producing Fe/Fe2+ electrodes at a rate of about 68.6 m2 per day. Additionally, we successfully assembled an Fe/FeCl2-Graphite battery at about a 0.42 ampere-hour level, paving the way for the scalable application of Fe/FeCl2-Graphite batteries.
研究领域:
能源材料
·
电化学
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yao Huang,Shufeng Zhao,Hui Liu,Rong Chen,Lei Zhao,Shan Liu
Abiotic Fe (II) oxidation widely occurs in the natural subsurface environment and engineered dynamic processes, which possibly impacts the growth of indigenous microbes. As previously discovered, the oxidation of aqueous Fe 2+ at neutral pH effectively inactivates iron-reducing bacteria Shewanella oneidensis strain MR-1 (MR-1). Herein, the impacts of co-existing iron mineral on the oxidation of aqueous Fe 2+ and the subsequent disinfection activity on MR-1 were investigated with siderite selected as a representative iron mineral in the subsurface environment. The oxidation rate of aqueous Fe 2+ and the amount of generated OH radical increased as the content of siderite increased, while the MR-1 inactivation was alleviated. An initial concentration of 2.0 × 10 6 CFU/mL MR-1 was inactivated by about 2.7 orders of magnitude during oxidation of 0.2 mM FeSO 4 alone for 30 min, which was reduced to only about 0.6 orders of magnitude in the presence of 4.3 mM co-existing siderite. ROS scavenging results confirmed that the OH radical generated in the bulk solution was not the leading role for the inactivation of MR-1. Morphological changes of the cells observed by SEM demonstrated that the disruption of the cell membrane was alleviated by siderite, which was further supported by the XRD and FTIR spectra. The underlying mechanism was proposed to be the reduced contact time of Fe 2+ and MR-1 cells due to the accelerated oxidation. This work provides new insights into the disinfection behavior of heterogeneous Fe (II) oxidation on iron cycling bacterial in the natural environment.
研究领域:
环境科学
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微生物学
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ACS Catalysis
·
2026
·Vol. 16
·期 20
·20616-20627
·
IF 13.6
Yuan Jingkang,Zhao Chao,Jin Yu,Hou Qilin,Cui Zhi,Tan Daolin,Ou Honghui,Yan Xiaoqing,Yang Guidong
The electrocatalytic co-reduction of nitrate (NO 3 − ) and carbon dioxide (CO 2 ) into urea represents a potential avenue for achieving efficient urea production. However, this process involves intricate C–N coupling reactions and faces a severe kinetic mismatch between the reduction pathways. This disparity typically leads to a disproportionate coverage of key C- and N-containing intermediates on the catalyst surface, resulting in dominant competitive side reactions. Herein, we report the design of a heterogeneous FeNi@AC catalyst that integrates isolated Fe single atoms and Fe–Ni dual-atom sites at the atomic scale, enabling the efficient conversion of NO 3 − and CO 2 into urea. Combined experimental and theoretical investigations reveal that the isolated Fe single-atom sites retain high nitrate reduction capability. Crucially, the introduction of Ni induces an electronic reconfiguration of the Fe center, which significantly lowers the energy barrier for CO 2 activation (from 0.7 eV to 0.1 eV). This activation effectively bridges the kinetic gap between C- and N-species. Consequently, the FeNi@AC catalyst achieves a urea yield rate of 13.6 mmol g –1 h –1 and a Faradaic efficiency of 51.7% at –0.8 V (vs RHE). This work not only presents an active catalyst for urea synthesis but also provides a site-specific regulation strategy for designing multifunctional atomic-site catalysts tailored for complex tandem reactions.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
·
IF 5.4
Chaobao Wang,Binlu Zhang,Jiale Chen,Yuanke Cai,Zihao Sun
Water-based lubricants are environmentally sustainable, but their inherently low viscosity is not conducive to the formation of stable lubricating films. To address this challenge, we propose a biomimetic strategy that integrates polydopamine (PDA) adhesion and hyaluronic acid (HA) hydration lubrication via Fe³ ⁺ coordination. The PDA-Fe³ ⁺-HA (PFH) ternary composite was prepared stepwise: Fe³ ⁺ coordinated with PDA catechol groups and interacted with HA chains through ionic crosslinking and chelation, thereby anchoring HA onto PDA. Tribological tests of UHMWPE/tin bronze tribopairs lubricated with the optimal PFH composite (mass ratio) showed that, compared with pure water, the average friction coefficient and wear rate decreased by up to 43.93% and 60.28%, respectively. The lubrication mechanism involves three synergistic effects: (i) Fe³ ⁺-enhanced PDA anchoring forms a stable adhesive layer; (ii) surface-exposed HA chains provide a hydrated low-shear lubrication layer; (iii) Fe³ ⁺ coordination bridges PDA and HA, integrating adhesion and lubrication functions. This bioinspired design offers an eco-friendly lubricant additive strategy. Download: Download high-res image (247KB) Download: Download full-size image
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CERAMICS INTERNATIONAL
·
2026
·
IF 6
Longgong Xia,Zhiqian Yu,Feng He,Yiwang Zhang,Huilan Yang,Kai Ma
(Fe/Zn/Ni)O·(Fe/Al) 2 O 3 spinels are widely used as raw materials for advanced ceramics and refractories and occur as precipitates in slag phases during nonferrous metal pyrometallurgy. The stability and phase-transformation mechanisms of these spinels are important for optimizing material performance and controlling metallurgical processes. The decomposition of Fe 3 O 4 , FeAl 2 O 4 , ZnFe 2 O 4 , ZnAl 2 O 4 , NiFe 2 O 4 , and NiAl 2 O 4 under various atmospheres was experimentally investigated, and phase evolution during reduction was elucidated. Thermogravimetric and differential thermal analyses and reduction experiments showed that Fe(II)-bearing spinels tended to decompose at elevated temperatures in air. ZnFe 2 O 4 and ZnAl 2 O 4 were stable at temperatures up to 1500 °C in air and in an atmosphere with p O2 = 10 −6 atm. At low oxygen partial pressure, aluminate spinels exhibited greater stability. The reduction kinetics of these spinels were also analyzed. The reduction of Fe 3 O 4 , ZnFe 2 O 4 , NiFe 2 O 4 , and NiAl 2 O 4 was described by the Avrami-Erofeev model, indicating that the reduction process was controlled by the nucleation rate. The reduction of ZnAl 2 O 4 was described by a diffusion model.
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