RSC Advances
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2017
·Vol. 7
·期 37
·22802-22809
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IF 3.108
Ruobai Li,Jing Kong,Haijin Liu,Ping Chen,Guoguang Liu,Fuhua Li,Wenying Lv
The degradation of indomethacin (IM) by ferrous ion-activated potassium peroxydisulfate (Fe2+/PDS) was investigated. We aimed to determine the optimal conditions for the removal of IM under different concentrations of Fe2+and PDS, evaluate the effects of operational parameters (solution pH, humic acid (HA), N2 bubbling and persulfate species), and propose the degradation mechanism of IM by the Fe2+/PDS system. The sequential addition of Fe2+ led to an improvement in the IM degradation and TOC removal efficiency. When the molar ratio of IM/PDS/Fe2+ was 1 : 1.5 : 2, the IM was almost completely degraded. Restrictions to the degradation efficiency of IM were caused by increasing the solution pH, bubbling with nitrogen, or through the addition of HA. A low concentration of Cl− had no effect on the reaction, while a high concentration led to a dramatic inhibitory effect. In addition, quenching experiments revealed that SO4˙− was the major active radical for the degradation of IM by ferrous ion-activated peroxydisulfate. Based on the identification of transformation products by liquid chromatography-mass spectrometry (LC-MS/MS), the pathways of the ferrous–peroxydisulfate oxidative system for the degradation of IM were tentatively proposed.
研究领域:
环境科学
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化学工程
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Xue-Meng Fan,Hou-Yong Yu,Duan-Chao Wang,Zhong-Hao Mao,Juming Yao,Kam Chiu Tam
A simple and eco-friendly Fe2+/H2O2 oxidation of microcrystalline celluloses (MCCs) to prepare cellulose nanocrystals (CNCs) with high carboxylation content is proposed. The effects of reaction times on the morphology, microstructure, and chemical and thermal properties of isolated carboxylated CNCs were investigated. The oxidative decomposition of Fe2+/H2O2 solution of MCC yielded CNCs with a size of 92–140 nm in length and 19–23 nm in width. The CNCs extracted at 6 h possessed the highest carboxyl content (2.2 mmol/g) with a zeta potential of −41 mV and a thermal decomposition temperature of greater than 325 °C. These CNCs are efficient adsorbents for dyes (methylene blue) and metal ions (copper ion) found in wastewater, with removal rates of up to 95.6 and 82.3%, respectively.
研究领域:
材料科学
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环境科学
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化学工程
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Hongji Chen,Yan Wu,Huiping Xiao,Hongfei Yin,Qian Fei,Chunyu Yuan,Qiuyu Zhao,Yujin Zhang,Yongzheng Zhang,Woonming Lau
Owing to the low conversion efficiency of Fe 3+ to Fe 2+ during the peroxymonosulfate (PMS) activation process, the design of an efficient Fenton-like catalyst is still a challenge. In this work, 0D/2D Co-doped Fe 2 O 3 /g-C 3 N 4 (CNCFO) composite catalysts were constructed for organic pollutant degradation, where the Co-doping not only boosts the conversion efficiency of Fe 3+ to Fe 2+ , but also acts as active site for PMS activation. Among them, CNCFO2 showed excellent catalytic performance, where 96.4% of MO could be degraded within 45 s. X-ray photoelectron spectroscopy (XPS) confirmed that the cobalt doping promoted the cycle of Fe 3+ /Fe 2+ , which was responsible for the enhanced PMS activation. Meanwhile, the good stability and reusability of CNCFO2 itself provide opportunities for its potential practical applications. Based on systematical characterizations, the Z-scheme photo-Fenton mechanism was proposed. This study offers a fresh perspective on the advancement of designing highly efficient Fenton-like catalyst for applications in the field of environmental purification.
研究领域:
环境科学
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催化材料
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高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 23
·4726-4734
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IF 6.331
Wenli Zhao,Guangpu Zhang,Yang Du,Shuangqin Chen,You Fu,Fan Xu,Xiangyun Xiao,Wei Jiang,Qingmin Ji
The proportion of Fe2+ and Fe3+ in Fe-based nanozymes is a key point in determining their catalytic activity. However, it is hard to adjust the Fe2+/Fe3+ ratio in nanozyme systems to achieve the best catalytic performance. In this work, we successfully regulate Fe2+/Fe3+ ratios in a wide range of 0.81–1.45 based on a novel porous platform of Fe doped silica hollow spheres. The homogeneous distribution and stable fixation of Fe components in Fe doped silica hollow spheres facilitate the valence regulation of Fe in the reduction heating in H2/Ar. When the Fe doped spheres (FeOx@SHSs) were used as nanozymes, different Fe2+/Fe3+ ratios have shown to influence the peroxidase-like catalytic activity greatly. The highest activity at the ratio of 1.41 should be due to the combined effects of the accelerated reaction rate by Fe2+ and the enhanced catalytic cycle efficiency by Fe3+. The FeOx@SHSs-based nanozyme is further applied to construct a facile colorimetric biosensing system, which exhibited extremely sensitive determination of glucose. This work presents an effective platform for controlling Fe valences and optimizing the peroxidase-like activity for catalytic processes or sensing systems.
研究领域:
材料科学
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分析化学
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生物传感
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DOI
PubMed
高影响因子
FOOD CHEMISTRY
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2020
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IF 6.306
Xianfeng Lin,Qianru Yu,Wei Yang,Chuxian He,You Zhou,Nuo Duan,Shijia Wu
Herein, a new double-enzymes-modulated fluorescent assay based on the quenching of upconversion nanoparticles (UCNPs) by Fe 3+ was constructed for sensitive determination of OPs. OPs can inhibit the activity of acetylcholinesterase to reduce the production of choline and further lead to the lack of H 2 O 2 in the presence of choline oxidase. Therefore, Fe 2+ cannot be converted into Fe 3+ , resulting in “turn-on” fluorescence of UCNPs. Under optimal conditions, an excellent linear correlation between the inhibition efficiency and the logarithm of the chlorpyrifos concentration was achieved with a detection limit (LOD) of 6.7 ng/mL in the range of 20–2000 ng/mL. The recovery for chlorpyrifos in apples and cucumbers was 89.5–97.1%. The results were consistent with those obtained by GC–MS. Overall, the integration of UCNPs into the double-enzymes-mediated Fe 3+ /Fe 2+ conversion endows this method with desirable rapidity, sensitivity, selectivity, stability, operational simplicity, and strong anti-interference capability, holding great potential in the application of food safety.
研究领域:
分析化学
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食品安全
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环境科学
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DOI
PubMed
高影响因子
International Journal of Analytical Chemistry
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2019
·
IF 1.682
Kai Sun,Qingzhu Liu,Rui Zhu,Qi Liu,Shunyao Li,Youbin Si,Qingguo Huang
Certain nano-scale metal oxides exhibiting the intrinsic enzyme-like reactivity had been used for environment monitoring. Herein, we evaluated the oxidase-mimicking activity of environmentally relevant nano-MnO2 and its sensitivity to the presence of metal ions, and particularly, the use of MnO2 nanozyme to potentially detect Cu2+, Zn2+, Mn2+, and Fe2+ in water. The results indicated the oxidase-like activity of nano-MnO2 at acidic pH-driven oxidation of 2,6-dimethoxyphenol (2,6-DMP) via a single-electron transfer process, leading to the formation of a yellow product. Notably, the presence of Cu2+ and Mn2+ heightened the oxidase-mimicking activity of nano-MnO2 at 25°C and pH 3.8, showing that Cu2+ and Mn2+ could modify the reactive sites of nano-MnO2 surface to ameliorate its catalytic activity, while the activity of MnO2 nanozyme in systems with Zn2+ and Fe2+ was impeded probably because of the strong affinity of Zn2+ and Fe2+ toward nano-MnO2 surface. Based on these effects, we designed a procedure to use MnO2 nanozyme to, respectively, detect Cu2+, Zn2+, Mn2+, and Fe2+ in the real water samples. MnO2 nanozyme-based detecting systems achieved high accuracy (relative errors: 2.2–26.1%) and recovery (93.0–124.0%) for detection of the four metal ions, respectively. Such cost-effective detecting systems may provide a potential application for quantitative determination of metal ions in real water environmental samples.
研究领域:
环境科学
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生物化学
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DOI
PubMed
高影响因子
CHINESE CHEMICAL LETTERS
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2015
·
IF 1.587
Xin-Ping Ouyang,Yun Yang,Guo-Dian Zhu,Xue-Qing Qiu
The lack of suitable lignin model compound limits the understanding of the characteristics of lignin, and hence hinders the efficient utilization of this kind of bioresource. A tetramer phenolic lignin model compound composed of 5-5, α - O -4 and β -5 linkages was prepared by a two-step of free radical reaction with hydrogen peroxide/horseradish peroxidase and S 2 O 8 2− /Fe 2+ as the initiator. Compared with enzymatic process, this synthetic process gives a higher yield of 33.8% within a shorter time. HRMS and 13 C NMR spectroscopy show that synthesized model compound contains phenylpropane structure linked by 5-5, α - O -4 and β -5 bonds, which can mimic some chemical characteristics of lignin.
研究领域:
生物化学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jawad Ali,Dan Li,Ajmal Shahzad,Muhammad Wajid Ullah,Jerosha Ifthikar,Muhammed Asif,Chen Yanan,Xie Lei,Zhuqi Chen,Songlin Wang
The Fe-based materials were considered very attractive for the treatment of wastewater using peroxymonosulfate (PMS) activation. However, the difficulties to restore the active Fe 2+ oxidation state restrict them to attained sustainable efficiency. In this work, a new strategy was introduced to accelerate the regeneration of Fe 2+ state through constructing an electron-rich MoS 4 2− centre in the inter-layers of FeMgAl layered double hydroxide (MoS 4 -LDH) catalyst. The dual centre MoS 4 -LDH catalyst was found more efficient as clear from the observed atrazine (ATZ) degradation rate of 0.117 min −1 , 100 times higher than the Fe 3+ /PMS or 25–50 times higher than the Fe based single centre NO 3 -LDH/PMS, CO 3 -LDH/PMS or S 2 O 4 -LDH/PMS systems, respectively. This boosted efficiency was related to the electron-rich MoS 4 2− centre which allows the constant electron transfer to reduce the electron-deficient Fe 3+ center at MoS 4 -LDH surface and thereby accelerating the Fe 2+ /Fe 3+ redox cycle during reaction. Furthermore, the MoS 4 -LDH/PMS system exhibited a broader effective pH (3.0–9.0), good stability and minimum influence of background electrolyte or organic matter. The degradation pathway of ATZ based on free radical (SO 4 – and OH), involving the redox cycles of Fe 3+ /Fe 2+ and Mo 6+ /Mo 4+ was proposed for the activation of PMS . This work highlighted the essential role of MoS 4 2− moiety, to accelerate the Fe 3+ reduction at the surface of the LDH catalyst through the continuous feeding of electrons.
研究领域:
环境科学
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催化化学
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高影响因子
JOURNAL OF HYDROLOGY
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2024
·
IF 5.9
Cui Gan,Zhaobo Luo,Chengyuan Su,Caixi Hu,Lei Tong,Jianbo Shi
The hyporheic zone is a crucial ecohydrological interface that plays a substantial role in the biogeochemical activity of iron and its mediated pollutant conversion. It is significantly influenced by dissolved oxygen and temperature fluctuations, but the combined effects and mechanisms are unknown. In this study, the co-transport behavior of goethite colloid (Goe), aqueous Fe 2+ and oxytetracycline (OTC) in groundwater discharge was simulated by column experiments. Our findings reveal that compared with room temperature (25 °C), the penetration rates of these compounds were generally promoted (0.1–7.0 % Goe, 14.1–43.1 % Fe 2+ , 0–19.6 % OTC) at low temperature (10 °C) but inhibited (0–5.0 % Goe, 0–51.0 % Fe 2+ , 0–3.8 % OTC) at high temperature (35 °C). At room temperature (25 °C), only 5 % of the Goe can penetrate the triadic transport system, where the Fe-OTC complex decreased the Zeta potential of Goe, hence improving its transport capacity. Compared with the penetration of individual Fe 2+ , the Fe 2+ transport was increased by 13.2 % due to the promoting effect of OTC on Fe redox cycling, whereas the electron transfer effect between Goe and Fe 2+ inhibited the transport by 46.6 %. The impact of μg/L OTC on the migration of Fe and Goe was dramatically diminished compared to the mg/L level. OTC was eliminated mainly by complex internal oxidation with Fe, weak adsorption, chemisorption, and hydroxyl degradation effects, but these were diminished at low temperatures while intensified at high temperatures. This study provides a deeper understanding of the intricate mechanisms of Fe and antibiotic transport in hyporheic zones, highlighting the significant roles of temperature and chemical interactions, particularly during seasonal changes.
研究领域:
环境科学
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生态学
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Shuyan Guan,Lulu An,Yumei Chen,Xianyun Liu,Jianchao Shi,Yulong Sun,Yanping Fan,Baozhong Liu
Highly active and stable non-noble metal catalysts are expected to play a critical role in future hydrogen storage and conversion applications. The design of active sites with composite oxides provides a new approach for developing high-performance catalysts. In this study, an Fe-doped Ni/NiO nanocomposite film was constructed on an ionic liquid/water interface to promote hydrogen generation. The optimized Ni/FeNiOx-25 catalyst showed excellent catalytic activity toward ammonia borane hydrolysis, with a turnover frequency of 72.3 min–1. The enhancing effect of Fe2+ doping on Ni/NiO films was confirmed by the improved intrinsic activity and theoretical simulations. Fe ion doping stabilized NiO and prevented NiO from becoming Ni. The interfacial Ni–Fe2+ dual active sites on the FeNiOx and Ni interfaces participated in the targeted adsorption and effective activation of water and NH3BH3 molecules, respectively. The sufficiently exposed plane surface of the nanofilms provided abundant active sites for catalytic reactions. This significant advance will inspire development in the ambient liquid hydrogen storage field.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 56
·85185-85201
·
IF 5.19
Chen Shiyao,Yan Caixia,Nie Minghua,Wu Leliang,Ding Mingjun,Wang Peng
This study evaluated the improvement of bisphenol A (BPA) elimination through hydrogen sulfite (HS) coupling with persulfate (PS) activated by low amounts of Fe 2+ . Under the optimum condition (10 μM Fe 2+ , 0.6 mM HS, 0.8 mM PS, pH = 4.0), 100% BPA (5 μM) was removed within 15 min. Sulfate radical (SO 4 •− ) and singlet oxygen ( 1 O 2 ) were confirmed as the primary active species for BPA degradation in the Fe 2+ /HS/PS system, and the steady-state concentration of SO 4 •− and 1 O 2 was 2.43 × 10 −9 M and 1.67 × 10 −9 M, respectively. Besides, FeHSO 3 + and FeOHSO 3 H + were the main iron species in the Fe 2+ /HS/PS system. The removal potency of BPA depended on the operation parameters, such as chemical reagent dosages, reaction temperature, and the solution initial pH. The impact of NO 3 − , SO 4 2− , and humic acid (HA) on BPA removal was negligible, whereas Cl − , HCO 3 − , and HPO 4 2− restrained BPA decomposition. Two injections of HS could improve the limitation of BPA degradation efficiency due to the rapid consumption of HS in the reaction process. The lower removal efficiency of BPA was observed in real water matrices than that in ultrapure water. Whatever, up to 58.1%, 66.3%, 68.1%, and 88.1% of BPA were removed from domestic wastewater, lake water, river water, and tap water within 10 min, respectively. In addition, the BPA degradation process was characterized by the 3D fluorescence spectra technique, which indicated the BPA oxidation intermediates also have fluorescence characteristics. Moreover, 6 intermediate products were identified, and the possible degradation pathways of BPA were proposed. Additionally, the Fe 2+ /HS/PS system also exerted an excellent performance for the removal of other representative organic contaminants including enrofloxacin, acid orange 7, acetaminophen, and phenol. All results indicated that the Fe 2+ /HS/PS system could be a promising method for organic pollutant removal.
研究领域:
环境科学
·
化学工程
·
水处理技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Hao Zheng,Jinlin Yin,Ping Lu,Yi Lu,Xinyan Jiang,Shaoke Chen,Yifei Pan,Ning Zhang,Jin Wang,Zhengquan Li
Fe 2+ -doped Cs 2 CuBr 4 induces strong spin polarization, resulting in efficient charge separation. • O 2 is efficiently activated through antiferromagnetic coupling upon spin-polarized Fe 2+ centers. • The optimized Fe-doped Cs 2 CuBr 4 enables highly efficient and selective photocatalytic oxidation of toluene to benzaldehyde. The high thermodynamic stability and spin-forbidden transition of ground-state triplet oxygen ( 3 O 2 ) to reactive species like superoxide radical (•O 2 − ) pose a formidable challenge for the photocatalytic oxidation of toluene. In this work, we introduced Fe 2+ active sites into Cs 2 CuBr 4 to achieve highly efficient and selective photocatalytic oxidation of toluene to benzaldehyde. The magnetic coupling between Fe 2+ and Cu 2+ breaks the intrinsic antiferromagnetic ordering of the lattice, significantly enhancing spin polarization. Crucially, this enhanced spin state not only facilitates the separation of photogenerated charge carriers but also directly drives the otherwise spin-forbidden conversion of 3 O 2 into reactive oxygen species ( e.g. , •O 2 − ). As a result, the Fe-doped Cs 2 CuBr 4 delivers a dramatically improved benzaldehyde production rate of 15.88 mmol g −1 h −1 (86.4% selectivity), far surpassing the pristine Cs 2 CuBr 4 (0.34 mmol g −1 h −1 ). More strikingly, the application of a 50 mT magnetic field triggers an additional boost to 27.23 mmol g −1 h −1 . This work highlights spin-polarization engineering as an effective strategy for advancing the efficiency and selectivity of photocatalytic oxidation systems. Download: Download high-res image (153KB) Download: Download full-size image
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