Journal of Materials Chemistry A
·
2014
·Vol. 3
·期 5
·2120-2127
·
IF 0
Fangyuan Gai,Tianlei Zhou,Yunling Liu,Qisheng Huo
In this study, a water-soluble Fe3+ ratiometric fluorescent sensor was designed and synthesized by encapsulating a donor–acceptor (D–A) dye 4-formacyl-triphenylamine (FTA) into silica cross-linked micellar nanoparticles (SCMNPs). The quenching of FTA-encapsulated SCMNPs (FTA-SCMNPs) on Fe3+ sensing was confirmed using the fluorescence titration method. FTA-encapsulated functionalized SCMNPs (FTA-NH2-SCMNPs and FTA-SO3H-SCMNPs) were synthesized to demonstrate the surface charge effect of nanoparticles on Fe3+ fluorescence sensing. The sensing ability of Fe3+ followed in this order: FTA-SO3H-SCMNPs > FTA-SCMNPs > FTA-NH2-SCMNPs, which indicates that particles with stronger negative charge have better sensing abilities. Moreover, linear correlation between the quenching intensity and lower concentration of Fe3+ was in accordance with the Stern–Volmer equation in FTA-SCMNPs and FTA-SO3H-SCMNPs. FTA-SO3H-SCMNPs showed good selectivity for Fe3+ detection. Because of the charge effect of functionalized SCMNPs on a dye-doped Fe3+ sensing system, these kinds of nanoparticles offered possibilities to construct sensing ability-enhanced fluorescence-quenching sensors by tuning the surface charge.
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ENERGY
·
2025
·
IF 9.4
Da Cui,Peng Zhang,Shuang Wu,Hon Man Luk,Yixi Wu,Bin Liu,Shuo Pan,Jingru Bai,Qing Wang,Xuehua Zhang
Oil shale has garnered significant attention as a supplementary energy source to traditional fossil fuels. In this study, we investigated the catalytic hydrothermal liquefaction (HTL) of shale oil sludge using three catalysts (Fe, Na 2 CO 3 , Ni/Al 2 O 3 ) and three combinations in pairs. The hydrothermal oil (HTO) yield, energy recovery (ER), and conversion rate (CR) of organic matters were comprehensively analyzed under six catalyst conditions. Both Fe + Na 2 CO 3 and Fe + Ni/Al 2 O 3 paired catalyst combinations achieved similar HTO yields of 28.43 % and 28.13 % along with ER values of 56.19 % and 57.94 % respectively. Moreover, these two groups achieved remarkably high CR values of 81.88 % and 81.02 %, respectively. The HTO from the Fe + Ni/Al 2 O 3 combination has the highest H/C ratio and the lowest O/C ratio at 1.682 and 0.032, respectively. Elemental composition, Fourier transform infrared spectroscopy (FT-IR), and gas chromatography-mass spectrometry (GC-MS) analyses of HTO were conducted in this study. The HTO produced by using Fe + Ni/Al 2 O 3 exhibited the most ideal distillation distribution, with fractions below diesel accounting for up to 96.94 %. Based on the catalytic functions of Fe, Ni, and Al 2 O 3 , six potential synergistic mechanisms of Fe + Ni/Al 2 O 3 were summarized. These mechanisms highlighted Fe + Ni/Al 2 O 3 's roles in promoting compound conversion pathways in HTO, ultimately revealing the synergistic catalytic mechanism.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Bin Zheng,Long Zhou,Chengjie Xue,Kuang Wang,Zhanqiang Fang
Oxalic acid-modified ball-milled zero-valent iron (OA-ZVI bm ) was employed to activate sodium chlorite (ClO 2 - ) for the removal of norfloxacin (NOR). The complete removal of 20 mg/L NOR was achieved within 60 min by the OA-ZVI bm /ClO 2 - process. Compared with the ZVI bm /ClO 2 - process which was the ball-milled zero-valent iron (ZVI bm ) activate sodium chlorite, the reaction activity of the OA-ZVI bm /ClO 2 - process was increased by 102.6 times. Through scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), electrochemical testing, and density functional theory (DFT) calculations, which has been confirmed that the introduction of oxalic acid can significantly increase the surface Fe(II) content of OA-ZVI bm , and accelerate the electron transfer rate of iron nuclei, thereby improve the efficiency of ClO 2 - activation for the removal of NOR. The role of various active species in NOR removal, which were •O 2 - , 1 O 2 , Fe(IV), ClO 2 , and •OH, was elucidated through free radical quenching experiments, electron paramagnetic resonance (EPR) spectroscopy, and quantitative detection of active species. These active species all participated in the reaction, while •O 2 - played a dominant role in the reaction because it could transform into other active species, such as (•OH, 1 O 2 ). Inorganic anions and natural organic matter have no significant effect on the removal of NOR in the OA-ZVI bm /ClO 2 - process. The protonation of oxalic acid ensured its good pH applicability range (pH = 2–11), thus exhibiting excellent performance in NOR removal in real water bodies. This further demonstrates that OA-ZVI bm prepared by oxalic acid ball milling modification is an efficient ClO 2 - activator, offering promising prospects for antibiotic removal technology.
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PubMed
高影响因子
ACTA MATERIALIA
·
2024
·
IF 8.3
Kun Wei,Jianhong Duan,Gaosheng Li,Huifen Yu,He Qi,Hao Li
Multi-phase NaNbO 3 (NN) exhibits high adjustability on the ordering of both polarization and oxygen octahedral tilt, becoming a perfect carrier to design heterogeneous structure for boosting comprehensive energy storage properties. To balance the energy storage density and efficiency, the coexistence of the relaxor antiferroelectric (AFE) with high polarization capability and the relaxor ferroelectrics (RFE) with high efficiency is designed in this work by introducing Sr 0.7 Bi 0.2 □ 0.1 Ti 0.75 Ta 0.2 □ 0.05 O 3 (SBTT) into NaNbO 3 -BiFeO 3 . As a result, an outstanding capacitive energy density ( W rec ) of 12.25 J cm −3 with a high η of 83 % can be achieved in NN-BF-SBTT ceramic, which can be identified as a novel heterogeneous coexisting structure with the crossover of high polarization capability in relaxor AFE and high efficiency in RFE in terms of high-resolution TEM. Furthermore, grain refinement and the dense structure inhibit the leak current, suppress the concentration of oxygen vacancy defects and raise the activation energy ( E a ), thus enhancing the E B . These excellent energy storage properties overcome the trade-offs between the two sets of parameters ( W rec - η , Δ P - E B ), offering a refreshing strategy for the development of high-performance ceramic capacitors.
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Water
·
2024
·Vol. 16
·期 24
·3658
·
IF 3
Jialin Chen,Yi Xie,Jun Xia,Xiaolin Zhang,Dong Chen
An advanced photochemical reduction system involving the UV/Fe(III)–oxalate system was developed for the reduction of nitrate (NO3−) to harmless N-gaseous species, primarily nitrogen (N2), by carbon dioxide radical (·CO2−) generated in the presence of dissolved oxygen (DO). Electron paramagnetic resonance (EPR) analyses confirmed the presence of both ·CO2−and ·OH radicals. Systematic investigations were conducted on various operational parameters, such as the initial Fe(III) concentration, oxalate concentration, and pH levels, to assess their impacts on the efficiency and products of NO3−reduction. Notably, solution pH played a significant role in influencing the NO3−reduction efficiency and the final products. At pH 2, approximately 75% of NO3−was converted into N2with an 80% selectivity. In the pH range of 3 to 5, a remarkable NO3−removal rate of about 90% was achieved. Furthermore, higher concentrations of Fe(III) (2 mM) and oxalate (10 mM) were found to enhance NO3−removal to 91.95% and 88.71%, respectively. The presence of DO increased the oxidative potential in the reaction system, subsequently enhancing the selectivity conversion of NO3−to N2. In summary, the UV/Fe(III)–oxalate system exhibits significant potential for effective removal of NO3−while achieving high selectivity for the production of N2in water remediation applications.
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CARBON
·
2025
·
IF 11.6
Bowen Yang,Longhui Zheng,Zhiwen Cheng,Maohong Fan,Jiming Hao,Qiang Ma
Phenol-polluted water poses significant risks, inflicting serious harm on both aquatic and terrestrial organisms. While Fenton and Fenton-like processes have been widely employed in wastewater treatment, their effectiveness is hindered by a major limitation: the sluggish cycle of Fe(III)/Fe(II). This slow cycle has become the Achilles' Heel of these methods, preventing their broader application. In this study, graphene oxide (GO) was introduced to facilitate the generation of Fe(II) from Fe(III), enhancing peroxydisulfate (PDS) activation for pollutant degradation. The Fe(III)/GO/PDS system demonstrated effective pollutant degradation capability with 100 % treatment efficiency (phenol = 10 mg L −1 , GO = 50 mg L −1 , Fe(III) = 0.2 mM, PDS = 1 mM, and initial pH of 3). The radical-mediated oxidation mechanism was proposed based on radical scavenger effects, oxidation products, and electron paramagnetic resonance spectra. The conversion of methyl phenyl sulfoxide (PMSO) to methyl phenyl sulfone (PMSO 2 ) indicated the formation of Fe(IV) in Fe(III)/GO/PDS system. To reveal degradation rules for multiple substrates, eighteen molecular descriptors were calculated using density functional theory (DFT) and correlated them with degradation rate constants ( k ). BO n , E B3LYP , and F (−) x emerged as significant parameters in this relationship. The Fe(III)/GO/PDS system demonstrated excellent reusability during the first five runs, effectively treating contaminants. However, its performance was hindered by kinetic retardation when certain anions, such as phosphate and bicarbonate, were present. These findings contribute to both scientific understanding and technical development of persulfate activation via the Fe(III)/Fe(II) cycle using carbonaceous materials, particularly for environmental remediation applications.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
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2024
·
IF 4.7
Zhang Xutao,Chen Weiliang,Li Xiangqi
Excellent photocatalytic performance and recyclability are crucial for the long-term use of the photocatalyst. In this study, 5 mol% Fe doped zinc oxide (ZF5), was freeze-dried with bacterial cellulose (BC)/sodium alginate (SA) solution to fabricate a novel composite aerogel capable of degrading methylene blue (MB) under visible light. Ca 2+ crosslinking and hydrophobic modifications were adopted to strengthen the aerogel skeleton and enhance the cycling photocatalytic activity, meanwhile, making the aerogel floatable persistently. The influences of pH, ZF5 dosage, and initial solution concentration on MB degradation were investigated. Benefiting from the synergy between the components and the combined modification, the optimum composite aerogel exhibits photocatalytic efficiency of up to 97.4% at an initial MB concentration of 20 mg/L within an irradiation time of 80 min. In addition, it exhibits a degradation efficiency of 79.7% even after 8 cycles, showing great potential in visible-light-driven degradation of MB.
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WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 5
·1-17
·
IF 3.8
Zhou Zhuyou,Ji Yufeng,Wang Yong,Liu Menghe,Xu Ying,Liu Ruijie,Yang Mingjie,Zou Congyang
In this study, the carbon-doped bimetallic organic framework C 60 /MIL-101(Fe,Cu) catalyst was prepared for the first time via solvothermal synthesis method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and a series of other instruments. At the same time, methylene blue (MB) was used as the target degradation material to investigate the catalytic performance of H 2 O 2 for MB degradation under visible light. The degradation experiment showed that the removal rate of C 60 /MIL-101(Fe,Cu) to MB reached 99.2% within 80 min. Furthermore, cyclic experiments demonstrated good stability and reusability of the catalyst. Finally, the degradation mechanism of the reaction was deduced by quenching experiment, UV–vis diffuse reflection and mott-Schottky plots. The results show that hydroxyl radical (·OH) and superoxide radical (·O 2 − ) play a major role in the degradation of MB during photo-Fenton process.
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CHEMOSPHERE
·
2024
·
IF 8.1
Lei Wu,Yuan Gao,Siwen Qiu,Zixuan Hu,Changbo Liu,Changsheng Yue,Jun Zhou
The porous and defective structure of biochar (BC) can accelerate surface electron transfer, promote the generation of more reactive oxygen species (ROS) by persulfate (PS), and effectively degrade organic pollutants in the soil. Electron transfer is a crucial link in this process, directly determining its oxidative degradation efficiency. In this study, using a novel strategy of enhancing electron transfer on the surface of BC by loading iron, three Fe-loaded BC activators (Fe-FeO x @BC, Fe 2 O 3 @BC and Fe 3 O 4 @BC) were synthesized to support the oxidative remediation of benzo( a )pyrene (BaP, Model compound of PAHs)-contaminated soil by PS. The results showed that Fe 3 O 4 @BC supported PS oxidation and remediation of BaP-contaminated soil had the best effect among the three BC-based activators, and the reuse effect was stable. Under the conditions of Fe 3 O 4 @BC addition of 1.00 wt%, PS addition of 0.75 wt%, reaction temperature of 35 °C, and solid-liquid ratio of 1:2.5, the removal rate of BaP in the soil reached the maximum of 93.84% at 120 min, and the soil toxicity was significantly reduced after remediation. The defect structure, conductive magnetic particles, and active functional groups on the surface of Fe 3 O 4 @BC were the key factors for activating PS to degrade BaP. With the combined action of the free radical pathway caused by ROS and the non-free radical pathway caused by 1 O 2 , electron transfer, and active functional groups, BaP was degraded to small molecules such as CO 2 and H 2 O, achieving rapid and efficient remediation of organic contaminated soil.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhouyang Ma,Jiawei Wu,Fuling Yang,Shuli Wang,Huan Wen,Ligang Feng
Given its initially low activity and difficulty in active phase formation, Fe site regulation is rarely touched in FeNi-based oxygen evolution reaction (OER) catalysts. Herein, the Fe sites regulation and activity deciphering are demonstrated by selective phase transformation taking nitrogen-doped carbon confined FeNi nanoparticles derived from Fe 2 Ni-MIL-MOF pyrolysis as an example; driven by the reduction atmosphere and Kirkendall effect assisted by melamine pyrolysis, some Fe and Ni sites were separated to form metallic Fe and FeNi alloy and the subsequent fluorination process induced the ionic compound FeF 2 formation rather than NiF 2 , offering a good platform to evaluate the influence of active Fe phase for OER catalysis. Theoretical calculations combined with ex-situ and in-situ spectral characterization techniques proved the complete convention of FeF 2 into a high-valent and reactive intermediate state of FeOOH. Considering the stable metallic state of Ni, the largely improved catalytic performance could be attributed to the Fe site regulation and the subsequent synergistic catalysis effect. Compared to the traditional iron-based catalyst, theoretically, the electronic structure of FeF 2 was more conducive to the active FeOOH phase formation and significantly lowered the reaction energy barrier for OER. By addressing the aforementioned problems, low overpotential and good stability for OER catalysts were realized. The current work showed valid proof of the FeNi-based catalysts regulation via Fe sites for energy-relevant catalysis reactions.
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Journal of Energy Storage
·
2024
·
IF 8.9
Yunxiao Jia,Bohao Peng,Xinyi Li,Shifang Huang,Xiaosong Zhang,Yulong Ding,Zhu Jiang
Low thermal conductivity is one of the key defects of pristine phase change materials (PCMs) for solar thermal energy storage. Biomass derived carbonaceous matrix, which could be recycled from wide sources, are favourable to incorporate with PCMs for solar thermal storage applications for their highly porous structure and decent thermal properties. Their unique structures get from the grown plants also endue them with diverse properties and functions, such as anisotropic thermal properties for directional heat transfer. However, direct pyrolysis of biomass generally produces amorphous carbonaceous structure that suffers insufficient thermal conductivity. Therefore, this work proposed a simple, rapid, and effective Fe graphitisation route to derive pine wood as graphitic matrix to synthesize multifunctional shape stabilized composite PCM. The Fe graphitisation process has induced the conversion of amorphous carbon to well-ordered graphitic structure. Further elevating the catalytic temperature contributes to a high graphitisation degree up to 89.53 %. With this Fe graphitisation route, the thermal conductivity of PCM composite at its longitudinal direction has increased from 0.545 W · m −1 K −1 to 1.846 W · m −1 K −1 . The solar absorptivity has reached up to 95.60 %. Besides, a high amount of PCM (∼72.26 wt%) was retained by the matrix, offering a high endothermic enthalpy up to 154.2 J/g. In the meantime, the aligned tubular structure of graphitic matrix leads to an anisotropic heat transfer behaviour, displaying a greater thermal conductivity along the longitudinal direction. Therefore, this study has provided a new approach to fabricate high-performance biomass derived graphitic matrix based PCM composite for solar thermal storage applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zekun Dong,Jiao Yang,Jie Yao,Yu Tang,Yan Zhang
Electro-peroxone (EP) is an emerging technology that combines electrochemistry and O 3 to remove contaminants. However, conventional carbon cathodes primarily contribute to the synthesis of H 2 O 2 in the system, which may scavenge HO . Herein, a series of Fe-based layered double hydroxides (LDH) was loaded onto graphite felt cathodes to strengthen the removal of organic contaminants. The EP system with CuFe-LDH/GF cathode (EP-CuFe-LDH/GF) demonstrated the highest removal rate (91.2 % within 20 min) of oxalic acid (OA), a typical ozone-resistance substance, approximately twice that of the EP-GF system. HO was identified the main reactive species. A new pathway for O 2 reduction and the generation of HO was found. The loading of CuFe-LDH altered the reduction pathway of O 2 on the GF cathode from 2e − to 1e − or 4e − process. As a result, HO was produced by the combination of O 3 and O 2 − instead of O 3 and H 2 O 2 , which avoided the quenching of HO by H 2 O 2 and enhanced the removal of OA. Moreover, the breaking complexation by O 3 , cathodic O 3 reduction and metal-OH catalyzed O 3 processes also contributed to the HO formation. Furthermore, the system could efficiently remove OA across a broad pH range of 3.0 to 9.0, addressing the poor performance of conventional EP systems under acidic conditions. Overall, the finding of this significant mechanism advances the understanding of organic pollutants removal and broadens the potential applications of EP system.
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