ENVIRONMENTAL POLLUTION
·
2022
·
IF 9.988
Yao Tang,Jibo Dou,Zhijiang Lu,Jianming Xu,Yan He
The sluggish Fe 3+ /Fe 2+ cycle was the rate-limiting step in the Fenton-like reaction, and metal-free carbonaceous materials are considered as emerging alternatives to solve this problem. However, the effect of carbon material properties on the distribution of reactive species remains poorly understood. This study investigated the possibility and mechanism of using biochar to accelerate the Fe 3+ /Fe 2+ cycle to overcome the low efficiency of Fe 3+ /persulfate (PS) catalytic oxidation of phenanthrene . More importantly, the contribution of reactive species in the reaction systems with the variation of biochar pyrolysis temperatures was quantitatively studied. The results showed that medium-temperature derived biochar (BC500) had the greatest ability to enhance the Fenton-like system compared to the low- and high-temperature (BC350/700), and the first-order rate constant achieved 5.2 and 35.7-fold increase against the biochar/PS and Fe 3+ /PS systems, respectively. Using electrochemical evidence, sulfoxide probe tests, and steady-state concentration calculations, radicals yields were found to rise and then reduce with decreasing pyrolysis temperature, while the nonradical contribution of Fe(IV) increased to 56.3%. Electron paramagnetic resonance, Boehm titration, and Raman spectroscopy unraveled that the enhanced effect of biochar resulted from itself persistent free radicals, phenolic-OH, and edge defects, which enabled electron transfer between Fe 3+ and biochar. Fe 2+ was thus continuously generated and effectively activated the PS. This work enables a better understanding of the Fe 3+ -mediated Fenton-like reaction in the presence of biochar and provides a sustainable green strategy for Fenton chemistry with potential applications.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2020
·
IF 6.306
Hao-Hua Deng,Kai-Yuan Huang,Meng-Jun Zhang,Zhi-Yan Zou,Ying-Ying Xu,Hua-Ping Peng,Wei Chen,Guo-Lin Hong
In recent years, gold nanoclusters (AuNCs) have received considerable attention as optical transducers in chemo/biosensors. Herein, a facile and efficient assay for NO 2 − has been successfully developed based on the fluorescence quenching of AuNCs co-modified by bovine serum albumin and 3-mercaptopropionic acid (BSA/MPA-AuNCs). In the presence of NO 2 − under acidic conditions, Fe 2+ can be readily oxidized and transformed to Fe 3+ , which can significantly suppress the fluorescence of BSA/MPA-AuNCs via non-radiative electron-transfer mechanism. The linear range and detection limit for this system were found to be 5–30 μM (r = 0.9975) and 0.7 μM, respectively. Other common anions and cations showed only very minor interference with the NO 2 − detection. Furthermore, the effectiveness of the proposed sensing strategy was validated by the demonstration of good performance in the determination of the amount of NO 2 − in ham samples, rendering it a powerful tool for the assessment of food security and water quality.
研究领域:
分析化学
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生物传感
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食品科学
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产品关联
DOI
PubMed
高影响因子
Small Methods
·
2022
·Vol. 7
·期 1
·2201266
·
IF 15.367
Mingjun Nan,Min Wu,Yuqin Liu,Lin Qiao,Huamin Zhang,Xiangkun Ma
Aqueous manganese-based flow batteries (AMFBs) have attracted great attention due to the advantages of low cost and environmental friendliness. Extending the cycle life of AMFBs has long been a challenging theme. The titanium-manganese single-flow batteries (TMSFB) are promising due to their special structure and electrolyte composition. However, TMSFB with high areal capacity faces capacity decay for unknown reasons. In this work, the capacity decay mechanism (accumulation and growth of MnO 2 ) is clarified by a homemade in situ microscope system. Given that, a redox mediator of Fe 2+ /Fe 3+ is specially designed to boost the areal capacity of TMSFB without side reaction. The directional promoting principle of the Fe 2+ /Fe 3+ is elaborated in detail. Fe 2+ chemically reacts with the residual MnO 2 to form Fe 3+ , which is reduced to Fe 2+ by the electrochemical reaction. And then Fe 2+ continues reacting with MnO 2 until MnO 2 is consumed completely. As a result, the TMSFB with the areal capacity of ≈55 mA h cm −2 can stably operate at a current density of 40 mA cm −2 , which is the highest areal capacity reported in aqueous manganese-based batteries. This work provides a new strategy for boosting the capacity of manganese-based batteries, shedding light on the improvement of other deposition-type batteries.
研究领域:
电化学
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能源材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2025
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IF 5.1
Ruipeng Shen,Min Li,Shuo Wang,Yu-Mo Zhang,Sean Xiao-An Zhang
Based on the dynamic coordination and dissociation of a leuco dye and Fe2+/Fe3+, we constructed an electrochromic system where the coloring unit and redox unit were separate. This electrochromic system combined the advantages of the stability of the metal ions and the color adjustability of the dyes. The electrochromic mechanism was found to be universal to multiple leuco dyes and the device showed an absorption change of 0.25 and a coloration efficiency of 192 cm2 C−1. Moreover, compared with our previous work, the cycle life was effectively improved (up to 4900 cycles), which was suspected to result from the smaller oxidizing potential of Fe2+. This approach to improve the cycle life of electrochromic devices may inspire further important results in the future.
研究领域:
材料科学
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化学
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产品关联
DOI
高影响因子
Engineering
·
2023
·
IF 12.8
Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao
Realizing fast and continuous generation of reactive oxygen species (ROSs) via iron-based advanced oxidation processes (AOPs) is significant in the environmental and biological fields. However, current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect, giving rise to the sluggish Fe 2+ /Fe 3+ cycle and low dynamic concentration of Fe 2+ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with MoS 2 to achieve ultra-efficient Fe 2+ regeneration (equilibrium Fe 2+ ratio of 82.4%) and remarkable stability (more than 20 cycles) via a circulating flow-through process. Unlike the conventional batch-type reactor, experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode, initiated by the convection-enhanced mass/charge transfer for Fe 2+ reduction and then strengthened by MoS 2 -induced flow rotation for sufficient reactant mixing, is crucial for oxidant activation and subsequent ROS generation. Strikingly, the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency. Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology, especially in large-scale complex wastewater treatment.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Polymers
·
2022
·Vol. 15
·期 1
·216
·
IF 4.967
Xinxin Wang,Xinyu Zu,Ting Wang,Yanan Zhao,Yan Liang,Xiaochen Wang,Qian Chai,Yunjuan Zhang,Hongzhong Chen,Hua Wang
Lactoferrin (LF) is an iron-binding glycoprotein with various biological activities that has been extensively used in food and medical applications. Several methods for detecting LF have been reported, but they still face challenges in terms of sensitivity and simplicity of detection. To achieve an accurate and efficient detection of LF, we developed a method for the determination of LF in lactoferrin supplements using carbon dots (CDs) fluorescent probes. The N, S-doped PPI carbon dots (N, S-PPI-CDs) were prepared using a protein (peanut protein isolate) and cysteamine as precursors. The prepared N, S-PPI-CDs exhibited intense blue fluorescence and good biocompatibility, while the fluorescence intensity of the N, S-PPI-CDs showed a good linear relationship with Fe2+/Fe3+concentration (0–2 μM). The N, S-PPI-CDs exhibited a high potential ability to rapidly detect Fe2+/Fe3+within 30 s, with a limit of detection (LoD) of 0.21 μM/0.17 μM. Due to the reversible binding of LF to Fe, the N, S-PPI-CDs showed a high sensitivity and selectivity for LF, with a limit of detection (LoD) of 1.92 μg/mL. In addition, LF was quantified in real sample LF supplements and showed a fluctuation in recovery of less than 2.48%, further demonstrating the effectiveness of the fluorescent N, S-PPI-CDs sensor.Keywords:N, S-PPI-CDs;fluorescence probe;biocompatibility;Fe2+/Fe3+detection;lactoferrin supplement detection
研究领域:
分析化学
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材料科学
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生物技术
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产品关联
DOI
PubMed
高影响因子
Advanced Healthcare Materials
·
2021
·Vol. 10
·期 19
·2100780
·
IF 9.933
Xin Meng,Fan Zhang,Huanling Guo,Chunyang Zhang,Hangtong Hu,Wei Wang,Jie Liu,Xintao Shuai,Zhong Cao
Smart theragnostic nanoplatforms exhibit great promise in clinical tumor treatment. The Fe-based Fenton reaction in tumor sites may generate reactive oxygen species to kill cancer cells with negligible side effects on normal tissues. However, its efficiency and duration are limited by the low intracellular concentration of H 2 O 2 , weak acidicity of tumor tissue, and low catalytic activity of conventional Fenton reagents. Herein, a facile strategy is proposed to efficiently overcome these obstacles. An efficient enzymatic/Fenton-starvation nanoreactor PMs loaded with glucose oxidase and perfluoropentane (PGPMs) is constructed through synthesizing methoxy-PEG-carboxymethy-modified iron (Fe 2+ /Fe 3+ )-based metal–organic frameworks (PMs), followed by loading glucose oxidase (GOx) and perfluoropentane (PFP). PGPMs accumulating in the tumor tissue exhibit tumor microenvironment-responsive biodegradable behavior and unusual catalytic activity for Fenton reaction advantageous over Fe 3+ -based MOFs. Meanwhile, encapsulation of GOx into PGPMs further significantly increases the catalytic activity for Fenton reaction and also induces starvation therapy. PGPMs also exhibit considerable capabilities of ultrasound and tumor microenvironment-responsive T2 MR imaging applicable for contrast-enhanced diagnosis. Both in vitro and in vivo studies demonstrate the great diagnostic and therapeutic potentials of this nanoreactor in tumor.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
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材料科学
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诊断成像
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Lingling Hu,Yuhong Liao,Dehua Xia,Fei Peng,Li Tan,Shaoyun Hu,Changshuo Zheng,Xiaolong Lu,Chun He,Dong Shu
A visible-light-driven photocatalytic fuel cell system integrating electro-Fenton process (EF-PFC), comprised of oxygen vacancies-rich rGO/BiO 1−x I photoanode and biomass-derived N-doped carbon (BNC) cathode, was developed to eliminate organic pollutant and generate electricity synchronously. The structure and properties of rGO/BiO 1−x I were characterized by means of XRD, SEM, TEM, solid-state EPR, FTIR, Raman, XPS, UV-vis DRS and PL spectra. The photoelectrochemical activity of rGO/BiO 1−x I was characterized by Mott-Schottky plots, photocurrent responses and EIS. The experimental results indicated that the introduced oxygen vacancies and graphene modification not only promoted the light-harvesting ability but also greatly improved the generation and transfer rate of charge carriers. Most importanly, BNC, acted as cathode, could efficiently reduce oxygen to H 2 O 2 , thus leading to more ·OH production in the presence of Fe 2+ . Simultaneously, the photogenerated electron could efficiently accelerate Fe 2+ /Fe 3+ redox cycling for continuous Fenton reaction and increasing electricity generation in synergistic EF-PFC system. Using formic acid as sacrificial fuel, approximately 68% removal efficiency was reached in rGO/BiO 1−x I-BNC EF-PFC system under visible light irradiation for 240 min while the photocurrent density ( J sc ) and the maximum power density ( P max ) were measured to be 133.18 μA cm −2 and 17.50 μW cm −2 . Furthermore, the radicals trapping experiments, hydrogen peroxide quantitative studies and ESR tests clearly revealed the mechanism of enhanced performance in rGO/BiO 1−x I-BNC EF-PFC system. Therefore, this engineered rGO/BiO 1−x I-BNC EF-PFC system with the cooperation of Fe 2+ /Fe 3+ redox is a promising means to eliminate organic pollutants and generate electricity synchronously.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Analysis and Testing
·
2022
·Vol. 6
·期 2
·111-119
·
IF 0
Guo Xin,Deng Xin-Chun,Zhang Ya-Qing,Luo Qin,Zhu Xiao-Kang,Song Yang,Song Er-Qun
Rapid and accurate detection of pathogenic bacteria of Staphylococcus aureus ( S. aureus ) is of importance in the field of clinical research and practical application. Herein, we report a magnetic relaxation switching (MRS)-based strategy for detecting S. aureus in complex samples via the assistance of signal amplification system of liposome. In this design, vancomycin (Van) modified 200 nm magnetic beads (MB 200 -Van) and biotinylated immunoglobulin (Biotin-IgG) were employed as capture probes for S. aureus which following labelled by biotinylated liposomes loading with glucose molecule (Biotin-liposome@Glu, BLGs) based on the affinity of biotin with streptavidin. The released glucose molecules combining with glucose oxidase generated Fe 3+ , causing transverse relaxation time ( T 2 ) signal change. The combination of dual recognition of S. aureus , liposome assisted signal amplification, and the MRS-based assay achieved direct and specific detection of S. aureus in blood and abscess samples. The as-proposed method for S. aureus assay in this study shows potential application for infectious diagnosis in clinical.
研究领域:
临床研究
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生物医学工程
·
分子诊断
·
传染病
✓ 已验证
产品关联
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2025
·
IF 12.1
Yangzi Shangguan,Ranhao Wang,Huan Tang,Shimao Deng,Qiushi Hu,Jiaxin Liang,Huiling Zhou,Xihan Chen,Hong Chen
Photocatalytic antibiotic degradation is an energy-efficient and environmentally friendly approach with the potential for large-scale application but is severely constrained by the lack of efficient and stable catalysts to produce reactive oxygen species (ROS). This research introduces a charge-ordered 3D Fe 3 S 4 -PUF composite integrated into a custom-built photocatalytic tandem continuous-flow cylinder reactor (TCCR) for antibiotic degradation. The system consistently achieves 100% tetracycline (TC) degradation efficiency with Fe 3 S 4 -PUF during 130 h of continuous operation, benefiting from the charge-ordered 3D Fe 3 S 4 -PUF framework and the TCCR design. Mechanism investigations reveal that the abundant Lewis basic ≡SH site and light-induced sustainable Fe 2+ /Fe 3+ redox cycling within Fe 3 S 4 facilitates the production of H 2 O 2 and ROS. Density functional theory (DFT) calculations indicate that Fe 2+ acts as an active site for capturing and activating O 2 , leading to either one-electron (O 2 →O 2 •− →H 2 O 2 →•OH) or two-electron transfer (O 2 →H 2 O 2 ) pathways. Meanwhile, photogenerated electron and the oxygen atoms in H 2 O 2 provide electrons to Fe 3+ , facilitating the reduction of Fe 3+ to Fe 2+ , thus elucidating the Fe 2+ /Fe 3+ redox cycling mechanism. Moreover, the 3D PUF structure enhances the mass transfer and pollutant-ROS interactions. The continuous-flow photocatalytic reaction validate the efficient antibiotic degradation of Fe 3 S 4 -PUF composite, suggesting its potential for implementation in large-scale antibiotic wastewater treatment systems.
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
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 23
·4726-4734
·
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
·
生物传感
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）