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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 29 ·13619-13625 · IF 3.3

Facile synthesis of a fluorescent probe based on a terbium-based metal–organic framework for selective detection of Fe(III) and Al(III)

Xuequan Jing,Jiaming Liu,Meina Guo,Guoliang Chen,Guoqing Ren,Jiarong Li,Haonan Qin,Zhangwei Yao,Yinhua Wan,Weijie Song,Huifeng Zeng,Feifei Yang,Da Zhao,Kang Hu

It is critical to detect Fe3+ and Al3+ rapidly and accurately due to their high risk to humans and the ecological environment. In this work, a kind of terbium-based metal–organic framework fluorescent probe (Tb-MOF) is facilely fabricated that displays ultra-high selective detection of Fe3+ and Al3+ over various coexisting ions (i.e. Mn2+, Co2+, K+, Ca2+, Na+, Mg2+, Cd2+, Cu2+, Fe2+, Zn2+, Ni2+, Pb2+ and Cr3+). The obtained Tb-MOF exhibits emission at 547 nm and possesses outstanding thermal, fluorescent and chemical stability. The Tb-MOF shows a ratiometric fluorescence signal for Al3+, and the detection limits for Fe3+ and Al3+ are 0.91 and 6.10 μM, respectively. Moreover, the fluorescence intensities and concentrations of Fe3+ and Al3+ have good linear relationships across wide concentration ranges. Furthermore, the quantifications of Fe3+ and Al3+ are achieved in complex tap and river water samples with good recoveries. This study offers a facile and efficient method of developing a fluorescent probe that possesses the ability to quantify Fe3+ and Al3+ in real environmental water samples.

研究领域: 分析化学 · 环境科学 · 材料科学
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Small · 2024 ·Vol. 20 ·期 27 ·2309541 · IF 13

The Z-Scheme MIL-88B(Fe)/BiOBr Heterojunction Promotes Fe(III)/Fe(II) Cycling and Photocatalytic-Fenton-Like Synergistically Enhances the Degradation of Ciprofloxacin

Tingting Liu,Kaiyue Hu,Yansheng Li,Yanhong Wang,Dongmei Han,Zhihua Wang,Fubo Gu

The Z-scheme MIL-88B/BiOBr (referred to as M x B y , whereas x and y are the mass of MIL-88B(Fe) and BiOBr) heterojunction photocatalysts are successfully prepared by a facile ball milling method. By adding low concentration H 2 O 2 under visible light irradiation, the Z-scheme heterojunction and photocatalytic-Fenton-like reaction synergistically enhance the degradation and mineralization of ciprofloxacin (CIP). Among them, M50B150 showed efficient photodegradation efficiency and excellent cycling stability, with 94.6% removal of CIP (10 mg L −1 ) by M50B150 (0.2 g L −1 ) under 90 min of visible light. In the M x B y heterojunctions, the rapid transfer of photo-generated electrons not only directly decomposed H 2 O 2 to generate · OH, but also improved the cycle of Fe 3+ /Fe 2+ pairs, which facilitated the reaction with H 2 O 2 to generate · OH and · O 2 − radicals. In addition, the effects of photocatalyst dosages, pH of CIP solution, and coexisting substances on CIP removal are systematically investigated. It is found that the photocatalytic- Fenton-like reaction can be carried out at a pH close to neutral conditions. Finally, the charge transfer mechanism of the Z-scheme is verified by electron spin resonance (ESR) signals. The ecotoxicity of CIP degradation products is estimated by the T.E.S.T tool, indicating that the constructed photocatalysis-Fenton-like system is a green wastewater treatment technology.

研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Efficient removal of petroleum hydrocarbons from soil by percarbonate with catechin-promoted Fe(III)/Fe(II) redox cycling: Activation of ferrous and roles of ·OH and ·CO3-

Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu

Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .

研究领域: 环境科学 · 土壤修复
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ADVANCED FUNCTIONAL MATERIALS · 2019 ·Vol. 29 ·期 36 ·1904056 · IF 15.621

Fe(III)-Porphyrin Sonotheranostics: A Green Triple-Regulated ROS Generation Nanoplatform for Enhanced Cancer Imaging and Therapy

Jing Zhu,Chengchao Chu,Dongsheng Li,Xin Pang,Huili Zheng,Junqing Wang,Yesi Shi,Yang Zhang,Yi Cheng,En Ren,Jingliang Cheng,Xiaoyuan Chen,Gang Liu

To address the urgent need for effective sonodynamic therapy (SDT), a facile and efficient strategy is developed for fabricating a new class of sonotheranostics. Herein, a Fe(III)-porphyrin nano-sonosensitizer is prepared by a one-step coordination synthesis, and then anchored with Bis(DPA-Zn)-RGD and manganese superoxide dismutase (SOD2) siRNA. Benefiting from the delicate interactions of the Fe(III)-coordinated nanoformulations, a highly potent sono/gene combinational therapy guided by fluorescence/magnetic resonance imaging is achieved. Importantly, this sonotheranostics significantly enhances the SDT effect of porphyrin through the cancer-targeted delivery capability and enhanced reactive oxygen species production via triple-regulated approaches, including down-regulation of SOD2, depletion of glutathione, and generation of Fenton reaction. This work opens up new perspectives for developing versatile sonotheranostics to overcome the clinical challenges of SDT.

研究领域: 纳米技术 · 癌症研究 · 诊疗学 · 生物医学工程 · 分子生物学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Enhanced phosphate pollutant removal from liquid via adsorption flotation strategy: Synergic effect of Fe(III)-fulvic acid carrier and CTAB

Wenjuan Wang,Yanfang Huang,Hongfei Ma,Lulu Kou,Bingbing Liu,Hu Sun,Shuzhen Yang,Guihong Han

Eutrophication of water bodies due to excessive phosphate release is becoming a serious issue. Herein, an Fe(III)-fulvic acid carrier with a synergistic effect with a surfactant was fabricated for the first time by a solvothermal method and evaluated for the removal of phosphate via an adsorption flotation strategy. This study indicated that the solvothermal method significantly improved the specific surface area, pore structure and active site distribution of the adsorption carrier and initially enhanced its adsorption performance. In addition, based on the synergistic effect of Fe(III)-fulvic acid and cetyltrimethylammonium bromide (CTAB), the competitive effect of surfactant and target ion in the adsorption flotation process was effectively broken. The theoretical maximum adsorption capacity of Fe(III)-fulvic acid increased from 169.205 ± 0.846 mg·g −1 to 274.725 ± 0.550 mg·g −1 after introducing CTAB, which was improved by 62.32% relative to the adsorption stage. FTIR and XPS analyses verified that the re-enhancement of the adsorption performance of the adsorbent carrier was mainly attributed to the chemisorption of CTAB with the carboxyl groups on the carrier surface, which intensified the electrostatic attraction and ligand exchange between the carrier and phosphate. Additionally, fractal and EDLVO theories revealed that CTAB could obviously improve the floatability of the carrier particles. Concurrently, the regeneration studies suggested that Fe(III)-fulvic acid possessed stable adsorption and flotation separation performance after three cycles. Overall, the Fe(III)-fulvic acid fabricated in this study not only realized the resource utilization of fulvic acid but also had practical application potential for the purification of oxyanions.

研究领域: 环境科学 · 水处理 · 化学工程 · 材料科学
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BIORESOURCE TECHNOLOGY · 2012 · IF 4.98

Synthesis of Fe3O4 poly(styrene–glycidyl methacrylate) magnetic porous microspheres and application in the immobilization of Klebsiella sp. FD-3 to reduce Fe(III)EDTA in a NOx scrubbing solution

Xiaoyan Wang,Zuoming Zhou,Guohua Jing

Magnetic poly(styrene–glycidyl methacrylate) porous microspheres (MPPM) with high magnetic contents were prepared by surfactant reverse micelles and emulsion polymerization of monomers, in which the well-dispersed Fe 3 O 4 nanoparticles were modified by polyethylene glycol (PEG) and oleic acid (OA) respectively. The characterizations showed that both of the OA–MPPM and the PEG–MPPM were ferromagnetic, however, the OA–MPPM was used to immobilize the bacteria for more advantages. Therefore, the effects of monomer ratio, surfactant, crosslinker and amount of Fe 3 O 4 on the structure, morphology and magnetic contents of the OA–MPPM were investigated. Then, the OA–MPPM was utilized to immobilize Klebsiella sp. FD-3, an iron-reducing bacterium for Fe(III)EDTA reduction applied in NO x removal. Compared with free bacteria, the immobilized FD-3 showed a better tolerance to the unbeneficial pH and temperature conditions.

CAS / MDL: 106-91-2
研究领域: 环境科学 · 微生物学 · 材料科学
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LUMINESCENCE · 2020 ·Vol. 35 ·期 8 ·1350-1359 · IF 1.855

Fe(III) bipyridyl or phenanthroline complexes with oxidase-like activity for sensitive colorimetric detection of glutathione

Liu Zhang,Yue Hou,Xiaoyan Guo,Wei Liu,Congcong Lv,Chunyang Zhang,Yan Jin,Baoxin Li

In this study, three types of Fe(III) bipyridyl or phenanthroline (Fe(III)-L 3 ) complex could directly catalyze 3,3′,5,5′-tetramethylbenzidine (TMB) to induce blue chromogenic changes without H 2 O 2 . Fe(III)-L 3 complex could induce a colour change in TMB directly after a short incubation time. Due to the high oxidase-like activity of the Fe(III)-L 3 complexes, superoxide anion radicals (O 2 •– ) were formed in solution. Intermediates radical involving oxo-iron species were then produced that oxidized TMB to its oxidation products (oxTMB), which had an absorbance maximum at 652 nm. Glutathione (GSH) could inhibit the oxidation reaction of the Fe(III)-L 3 complex–TMB system, a rapidly colorimetric method was established for the specific detection of GSH that had a detection limit of 0.1 μM. Furthermore, Fe(III)-L 3 complexes could catalyze TMB to oxTMB directly without H 2 O 2 . This fast and simple colorimetric method may open a new avenue for application in the point-of-care diagnosis field using the TMB chromogenic system.

研究领域: 分析化学 · 生物化学 · 医学诊断
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ENVIRONMENTAL RESEARCH · 2024 · IF 7.7

Enhanced oxidative degradation of 2,4-dichlorophenol by iron oxychloride supported on graphitic carbon nitride via peroxymonosulfate activation: Significant role of Fe(II)/Fe(III) conversion cycle

Bin Nie,Haojun Dong,Jincan Yan,Shengyu Zhang,Shuang Zhong

The activation of peroxymonosulfate (PMS) by heterogeneous catalysts presents an exciting but challenging strategy for degrading persistent organic pollutants in water. Iron oxychloride (FeOCl) is considered a promising heterogeneous catalyst due to its unique oxygen bridge structure, which could render it more active by facilitating the iron valence transitions between Fe(II) and Fe(III). However, the limited Fe(II)/Fe(III) conversion cycle rate hinders its catalytic activity, leading to unsatisfactory PMS activations in practical applications. Herein, we demonstrated the performance and the mechanistic pathway of enhanced FeOCl (CNFeOCl) catalytic activation using a graphitic carbon nitride (g-C 3 N 4 ) with a unique electronic structure as a carrier employing 2,4-dichlorophenol (2,4-DCP) as a representative pollutant. The CNFeOCl/PMS system achieved complete degradation of 2,4-DCP (30 mg/L) in a short time (<5 min), whereas the FeOCl/PMS system degraded only 35.98% under the same conditions. The high 2,4-DCP degradation rate of CNFeOCl was due to its improved Fe(II)/Fe(III) ratio (34.34%/40.03%), increased specific surface area (30.32 m 2 /g), and reduced charge-transfer resistance. Combining a series of characterizations, electron spin resonance (ESR) detection, and quenching experiments, the investigations elucidated the enhanced catalytic activation mechanism of CNFeOCl which includes dominant reactive oxygen species (ROS) generation and some key factors that generally affected the efficiency of oxidative degradation. We believe this study offers new insights into the intrinsic role of g-C 3 N 4 supported FeOCl for PMS activation and provides theoretical support to guide the rational design for developing efficient iron-based catalysts toward heterogeneous catalysis.

CAS / MDL: 98-00-0
研究领域: 环境科学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Simultaneous removal of nitrobenzene, benzoic acid, flunixin meglumine and aspirin by CaO2/Fe(III) system: Enhanced degradation by crystal boron

Chaoqun Tan,Wangqi Yu,Hong Mei,Kaiyang Chen,Tianhui Xu,Huiming Xiang,Yiming Feng,Lin Deng

In this study, Fe(III) catalyzed calcium peroxide (CaO 2 , CP) Fenton-like process assisted by crystal boron (C-boron) was applied for in situ chemical oxidation. Flunixin meglumine (FMME), aspirin (ASA), nitrobenzene (NB) and benzoic acid (BA) were selected as target contaminants. Pollutants decomposition by the CP/Fe(III) and C-boron/CP/Fe(III) systems was proposed in terms of diverse parameters, including C-boron dosage, pH, and temperature, with regard to the pseudo-first-order kinetic model (R 2  > 0.95). About 26.8% of 20 μM FMME was removed by 0.5 mM CP and 0.5 mM Fe(III) after 20 min at pH 4.0, whereas 90.4% of FMME was decomposed in the C-boron/CP/Fe(III) system with 100 mg/L C-boron. The removal rates of the other three pollutants were also improved to varying degrees. The k obs of the C-boron/CP/Fe(III) system for these four pollutants degradation at pH 4.0 was approximately 4.1 ∼ 5.3 times higher compared to the CP/Fe(III) system. Electron paramagnetic resonance and quenching experiments indicated that OH, O 2 − and 1 O 2 were present in both systems and contribution of OH was 71.3% at initial pH 4.0 in C-boron/CP/Fe(III) system, suggesting that it was the main reactive oxygen species for the contaminants elimination. Furthermore, experiments on the characterization of C-boron showed great reactivity and stability. This work manifested the promotion mechanism of pollutant degradation in the C-boron/CP/Fe(III) system.

研究领域: 环境科学 · 化学工程 · 水处理
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ACS Biomaterials Science & Engineering · 2022 · IF 5.395

Fe(III)-Doped Polyaminopyrrole Nanoparticle for Imaging-Guided Photothermal Therapy of Bladder Cancer

Heng Liu,Mengsi Zhang,Hao Jin,Kepeng Tao,Chao Tang,Yanpeng Fan,Shuwei Liu,Yi Liu,Yuchuan Hou,Hao Zhang

Clinically, the surgical treatment of bladder cancer often faces the problem of tumor recurrence, and the surgical treatment combined with postoperative chemotherapy to inhibit tumor recurrence also faces high toxicity and side effects. Therefore, the need for innovative bladder cancer treatments is urgent. For the past few years, with the development of nano science and technology, imaging-guided therapy using nanomaterials with both imaging and therapy functions has shown great advantages and can not only identify the locations of the tumors but also exhibit biodistributions of nanomaterials in the tumors, significantly improving the accuracy and efficacy of treatment. In this work, we synthesized Fe(III)-doped polyaminopyrrole nanoparticles (FePPy-NH2 NPs). With low cytotoxicity and a blood circulation half-life of 7.59 h, high levels of FePPy-NH2 NPs accumulated in bladder tumors, with an accumulation rate of up to 5.07%ID/g. The coordination of Fe(III) and the amino group in the structure can be used for magnetic resonance imaging (MRI), whereas absorption in the near-infrared region can be applied to photoacoustic imaging (PAI) and photothermal therapy (PTT). MRI and PAI accurately identified the location of the tumor, and based on the imaging data, laser irradiation was employed accurately. With a high photothermal conversion efficiency of 44.3%, the bladder tumor was completely resected without recurrence. Hematological analysis and histopathological analysis jointly confirmed the high level of safety of the experiment.

CAS / MDL: 765-39-9 10025-77-1
研究领域: 纳米技术 · 癌症治疗 · 医学成像 · 生物医学工程
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NANOTECHNOLOGY · 2019 ·Vol. 31 ·期 1 ·015101 · IF 3.399

Encapsulation of glucose oxidase in Fe(III)/tannic acid nanocomposites for effective tumor ablation via Fenton reaction

Keke Du,Qianqian Liu,Mei Liu,Rongmu Lv,Nongyue He,Zhifei Wang

Increasing the content of reactive oxygen species (ROS) with the assistance of nanoformulations in cancer cells via the Fenton reaction is considered an effective method to treat cancer. However, the efficiency of the Fenton reaction is affected by the level of H2O2, the selection of iron ions in different nanoformulations, etc. Herein, we use FeIII-tannic acid (FeIIITA) nanocomposites as the carrier to deliver glucose oxidase (GOD) which can solve the problem of insufficient endogenous H2O2 by catalytically converting the glucose. In comparison with traditional Fe2+/Fe3+, FeIIITA nanocomposites perform higher catalytic activity in converting H2O2 to high toxic hydroxyl radicals (·OH) due to the TA-mediated reduction of Fe3+. So, the integration of GOD and TA in the construction of nanocomposites significantly enhances the efficiency of the Fenton reaction. In vitro experiments show that ·OH produced by GOD-FeIIITA nanocomposites can not only achieve a good anticancer effect at a low concentration but also promote degradability of the nanocomposites. When it is only 1.08 μg · ml−1, the cell apoptosis rate has reached 76.91%. In vivo experiments further demonstrate that GOD-FeIIITA nanocomposites can significantly inhibit tumor growth. So this work lays a good foundation for Fenton reaction-based cancer treatment.

CAS / MDL: 9001-37-0
研究领域: 癌症治疗 · 纳米技术 · 生物医学工程 · 化学生物学
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JOURNAL OF FLUORESCENCE · 2019 ·Vol. 29 ·期 3 ·769-777 · IF 1.913

Fluorescent Carbon Quantum Dots with Fe(III/II) Irons as Bridge for the Detection of Ascorbic Acid and H2O2

Luo Kuan,Jiang Xinyu

Nitrogen-sulfur co-doped carbon quantum dots (N, S-CQDs) with good photoluminescence properties were prepared by hydrothermal method using citric acid (CA) and methionine (Met) as precursors. Co-doping with N and S facilitates the electron transfer rate and coordination interaction between N,S-CQDs and Fe(III) ions which acts as a quencher of fluorescence. Based on a simple redox principle, a highly sensitive and selective method for the detection of ascorbic acid (AA) and H 2 O 2 was successfully developed. The calibration curves obtained are linear for the current versus AA and H 2 O 2 concentration over the range 50–500 μM and 10–140 μM, respectively. And the detection limits for AA and H 2 O 2 are 4.2 μM and 1.9 μM, respectively. The quantitative analysis of AA and H 2 O 2 in various juices and H 2 O 2 disinfectant with Fe 3+ /CQDs or Fe 2+ /CQDs gave the recoveries of 87.8%–117.5% and 99.2%–106.4% with relative standard deviations ( RSD ) of 1.6–5.1% and 1.7–3.1%, respectively, showing satisfactory results for the determination of AA and H 2 O 2 in actual application. The proposed strategy may provide a new pathway to developing inexpensive and sensitive way for the detection of various redox reaction–involved system.

研究领域: 分析化学 · 材料科学 · 生物化学
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