ACS ES&T Engineering
·
2022
·
IF 0
Kunjie Hou,Zhoujie Pi,Fei Chen,Li He,Fubing Yao,Shengjie Chen,Xiaoming Li,Haoran Dong,Qi Yang
The practical application of the traditional Fenton system (Fe(II)/H2O2) is seriously hampered by the sluggish Fe(III)/Fe(II) cycle and the stringent acidic reaction condition. In this work, we found that trace-dissolved S(-II) (DS(-II), 5 μM) could significantly accelerate the Fe(III)/Fe(II) cycle and trigger a rapid H2O2 activation process in the Fe(III)/H2O2 system. Thus, more hydroxyl radicals (·OH) were generated for the rapid removal of various organic pollutants such as bisphenol A (BPA) and sulfamethoxazole (SMX) from water. Besides, the additive DS(-II) effectively broadened the application pH range of the Fenton or Fenton-like system. The constructed Fe(III)/DS(-II)/H2O2 system showed extensive applicability to different water matrices and maintained high BPA removal in the actual water sources. Furthermore, the toxicity assessment revealed that the toxicity of the target contaminant was diminished. The harmless SO42– was the final product of DS(-II) in the Fe(III)/DS(-II)/H2O2 system, and the residual DS(-II) was less than the threshold limit value for fresh or saltwater (0.5 mg/L). This discovery is expected to promote the large-scale practical application of iron-based Fenton or Fenton-like systems in practical organic wastewater purification.
研究领域:
环境科学
·
水处理
·
污染控制
✓ 已验证
DOI
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Jingmin Wang,Xiaolong Hu,Haizhen Ding,Xin Huang,Mingsheng Xu,Zhenzhen Li,Dong Wang,Xu Yan,Yang Lu,Yunjun Xu,Yan Chen,Paulo Cesar Morais,Yupeng Tian,Ren-Quan Zhang,Hong Bi
Commercial gadolinium-based materials have been widely used as contrast agents for magnetic resonance imaging (MRI), but the high toxicity of leaking free Gd3+ ions still raises biosafety concerns. Here, we develop a novel, safe, and efficient MRI contrast agent based on a stable Fe(III) complex of fluorine and nitrogen co-doped carbon dots (F,N-CDs) that was prepared from glucose and levofloxacin by a simple microwave-assisted thermal decomposition method. The obtained Fe3+@F,N-CD complex exhibits higher longitudinal relaxivity (r1 = 5.79 mM–1·s–1) than that of the control samples of the Fe3+@CD complex (r1 = 4.23 mM–1 s–1) and free Fe3+ (r1 = 1.59 mM–1 s–1) in aqueous solution, as assessed by a 1.5 T NMR analyzer. More importantly, the Fe3+@F,N-CD complex is very stable with a large coordination constant of 1.06 × 107 in aqueous medium. While incubated with HeLa cells, the Fe3+@F,N-CD complex shows clear MR images, demonstrating that it has potential to be an excellent MRI contrast agent. Furthermore, in vivo MRI experiments indicate that the Fe3+@F,N-CD complex provides high-resolution MRI pictures of 4T1 tumor bearing BALB/c mice 15 min after injection and can be completely excreted 2 h after administration. No cytotoxicity was observed with F,N-CDs and Fe concentration up to 0.2 mg/mL and 0.3 mM in 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide cell proliferation assay, respectively. The possible mechanism of the enhanced MRI effect of the Fe3+@F,N-CD complex is therefore proposed. The extremely low toxicity, high r1 relaxivity, strong photoluminescence, and low synthetic cost enable the Fe3+@F,N-CD complex to be a safe and promising T1-weighted MRI contrast agent for clinical applications.
研究领域:
材料科学
·
医学影像
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yanjing Wang,Minglei Song,Jianrong Wei,Jie You,Siping Chen,Shuangyin Wang,Yanyong Wang
Electrochemically mediated Fe(II)/Fe(III) redox-coupled uranium extraction can efficiently reduce the cell voltage of electrochemical uranium extraction (EUE). How to regulate the surface structure to enhance the uranium acyl ion adsorption capacity and strengthen the Fe(II)/Fe(III) redox cycle process is crucial for EUE. In this work, we developed surface sulfated nanoreduced iron (S-NRI) for EUE and exhibited improved properties for EUE at an ultralow cell voltage (−0.1 V). Compared with a nanoreduced iron (NRI) adsorbent, S-NRI displayed faster electrochemical extraction kinetics properties and higher extraction efficiency and capacity for uranium. In a more complex seawater electrolyte containing uranyl ion concentration ranging from 1 to 20 ppm, the removal efficiency could reach almost ∼100% after EUE for 24 h. At a higher 50 ppm uranium acyl ion concentration in a seawater electrolyte, S-NRI exhibited higher extraction capacity (755.03 mg/g), which is better than 528.53 mg/g of NRI at a cell voltage of −0.1 V. Outstanding EUE property could be attributed to the fact that sulfate species (M–SO42–) on the S-NRI surface not only enhanced selective adsorption of uranyl ions but also strengthened the Fe(II)/Fe(III) redox cycle, which accelerated electron transfer between Fe(II) and U(VI), promoted the regeneration of Fe(II) active sites, and finally enhanced the EUE property.
研究领域:
材料科学
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环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Jiangdong Dai,Zhongshuai Chang,Atian Xie,Ruilong Zhang,Sujun Tian,Wenna Ge,Yongsheng Yan,Chunxiang Li,Wei Xu,Rong Shao
The research of superhydrophilic interface is developing rapidly, but the preparations of superhydrophilic surfaces through simple methods are still challenging. Herein, we reported a facile, rapid and environmentally-friendly approach for preparing a novel superhydrophilic and underwater superoleophobic membrane via the thermal oxidation of Cu mesh and one-step coordinated assembly of Fe(III)-CMC chelate hydrogel. Superhydrophilicity was attributed to the hydrophilicity of Fe(III)-CMC chelate hydrogel and nanoneedle-like rough structure of CuO@Cu membrane. The membrane was used to separate a variety of oil/water mixtures and exhibited excellent separation performance. Moreover, the membrane exhibited the excellent durability and superior stability against corrosion conditions. We envision that the Fe(III)-CMC@CuO@Cu membrane with good underwater superoleophobicity could provide a candidate not only for oil/water separation but also many other potential applications such as underwater oil manipulation, self-clean, and bio-adhesion control.
研究领域:
材料科学
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环境科学
·
界面化学
✓ 已验证
产品关联
DOI
高影响因子
Soft Matter
·
2018
·Vol. 14
·期 43
·8764-8770
·
IF 3.709
Botian Li,Da Xiao,Dongsheng Deng,Haimu Ye,Qiong Zhou,Liming Tang
In this study, a novel self-assembled metal–organic gel was synthesized from ferric nitrate and a di-topic ligand, bis(3-pyridyl)terephthalate. The gel consisted of a three dimensional network of uniform nanofibers. The gelation exhibited high selectivity to Fe(III) based on metal–ligand coordination. The molar ratio of Fe3+ to ligand had a large influence on the assembly process and the morphology of the gel. The metallogel displayed multi-stimuli responsiveness and excellent heat resistance, thus was further applied as a thermo-stable template for the polymerization of N,N′-methylene bisacrylamide to produce the core/shell polymer composite nanowires. Subsequently, the polymer nanotubes were obtained after ammonia post-treatment, comfirming the feasibility of the template synthesis strategy. According to the rheological measurements, the gel-like products of the composite nanowires exhibited better mechanical strength compared to the gel template.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF INORGANIC BIOCHEMISTRY
·
2021
·
IF 4.155
Yueqin Li,Changhao Qian,Yun Li,Yong Yang,Dong Lin,Xiaohui Liu,Chen Chen
Two novel Fe(III) complexes, Fe(HL 1 ) 2 Cl·1.25H 2 O ( 1 ) and Fe(HL 2 ) 2 ·Et 3 NH·H 2 O ( 2 ) (H 2 L 1 = o -vanillin benzoylhydrazone, H 3 L 2 = o -vanillin salicylhydrazone) are prepared. X-ray single crystal diffraction confirms that the hydrazone ligands can be chelated to iron centre resulting in a six-coordinate octahedral configuration. Both complexes show major intercalation effect to the herring sperm deoxyribonucleic acid (HS-DNA) with high binding constants of 2.01 × 10 4 M −1 and 2.24 × 10 4 M −1 , respectively. Molecular docking studies reveal both complexes can intercalate at the gap of DC5-DG2 and DG6-DC1 base pairs of DNA hexamer (1Z3F). The interaction of the complex 1 with plasmid pBR322 DNA induces distinguishable alterations of the DNA morphology. Further, the structure of plasmid pBR322 DNA treated with complex 1 in the presence of ascorbic acid has been damaged probably due to the reactive oxygen species (ROS) generation. What's more, both complexes show high affinity with bovine serum albumin (BSA), the binding constants measured by fluorescence techniques are 5.75 × 10 6 M −1 and 4.39 × 10 7 M −1 , respectively. Molecular docking demonstrates that the complexes prefer the binding pocket of site III (subdomain IIB) of BSA (PDB ID: 4F5S ). Similarly, dynamic light scattering (DLS) reveals that the complexes not only bind to BSA but also induce bigger size aggregates as the concentration increases.
研究领域:
无机化学
·
生物化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Jinwen Li,Qingcai Chen,Tong Sha,Yongchun Liu
Metal ions are key components in atmosphere that potentially affect the optical properties and photochemical reactivity of atmospheric humic-like substances (HULIS), while this mechanism is still unclear. In this study, we demonstrated that atmospheric HULIS coupled with Fe3+, Cu2+, Zn2+, and Al3+ exhibited distinct optical properties and reactive intermediates from that of HULIS utilizing three-dimensional fluorescence spectroscopy and electron paramagnetic resonance spectroscopy. The HULIS components showed light absorption that increased by 56% for the HULIS-Fe3+ system, fluorescence blue shift, and fluorescence quenching, showing a certain dose–effect relationship. These are mainly attributed to the fact that the highly oxidative HULIS chromophores have a stronger complexing ability with Fe3+ ions than the other metal ions. In addition, triplet organics (promoting ratio: 53%) and reactive oxygen species (promoting ratio: 82.6%) in the HULIS-Fe3+ system showed obvious generation promotion. Therefore, the main assumption of the photochemical mechanisms of atmospheric HULIS in the HULIS-Fe3+ system is that Fe3+ ions can form 3HULIS*-Fe3+ complexation with photoexcited 3HULIS* and then transition to the ground state through energy transfer, electron transfer, or nonradiative transition, accompanied by the formation of singlet oxygen and hydroxyl radicals. Our results provide references for evaluating the radiative forcing and aging effect of metal ions on atmospheric aerosols.
研究领域:
环境科学
·
大气化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Jinjuan Xue,Meng Yuan,Jiamin Gao,Zewu Zhang,Mingxin Wang,Shuaishuai Ma
In this work, a novel PCN-222 metal−organic framework based multitasking membrane was developed for separation of emulsified oils as well as photo-Fenton degradation of refractory aromatic pollutants and inactivation of pathogenic bacteria in water. Fe(III)@PCN-222 nanorods were prepared via impregnation method and subjected to amino-modification, and then robustly anchored on polydopamine (PDA) decorated PVDF membrane via catechol-amine reaction. The as-prepared N-Fe(III)@PCN-222/PDA/PVDF composite membrane exhibited underwater superoleophobicity, and showed high separation efficiency (above 99.4 %) as well as relatively favorable permeation flux (874.9–1592.3 Lm −2 h −1 ) in the separation of emulsified oils ranged from nanoscale to microscale from water. Meanwhile, the membrane serving as a recyclable photo-Fenton platform showed an extensive degradation capacity towards aromatic contaminants and high inactivation activity against bacteria under visible light. The grafted Fe(III) is used as an electron acceptor to promote the separation of photo-generated charge carriers, adjusted the band structure to shorten the bandgap value, and can be reduced to Fe(II) by photo-generated electrons as a Fenton-like catalyst. The photo-Fenton mechanism was studied in detail from the aspects of photoelectric properties, band structure and reactive oxygen species . This work could promote the application of PCN subclass MOFs based superwetting membrane as a recyclable platform for complex wastewater treatment .
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yu Chen,Yajing Li,Yongjian Wang,Igor Ying Zhang,Rongfu Huang
This work investigated the activation of peroxymonosulfate by electrochemical (EC) system assisted with Fe(III)-nitrilotriacetic acid (NTA) complex for degradation of persistent naphthenic acids (NAs) under neutral initial pH conditions. As NAs are a complicated mixture, 1-adamantanecarboxylic acid (ACA) was selected as the model NA compound for degradation experiment. The addition of NTA is to chelate with Fe(III), gaining stability under neutral pH condition to facilitate the circulation of Fe(II)/Fe(III) by the electrochemical process to activate PMS. The EC/Fe(III)-NTA/PMS system was explored with applicable pH range of 3–9 and an optimized molar ratio 1: 2 for Fe: NTA. Results of quenching and chemical probe experiment together with results of electron paramagnetic resonance (EPR) analysis revealed the main reactive species of the system, including • OH, SO 4 •− , 1 O 2 and possibly Fe(IV). With the addition of NTA, the yields of • OH, SO 4 •− , 1 O 2 were enhanced. Results of mass spectrometry analysis and DFT calculations indicated the formation of 9 degradation byproducts of ACA via three primary degradation pathways such as hydroxyl substitution, carbonyl substitution, and decarboxylation . Furthermore, the EC/Fe(III)-NTA/PMS system could achieve excellent removal efficiency of ACA with different anions such as Cl - , HCO 3 - , NO 3 - and H 2 PO 4 - in the background. The practical applicability of the system was also verified with the high removal of commercial NAs mixture standard. Overall results have indicated the EC/Fe(III)-NTA/PMS system could be utilized for efficient reclamation of authentic oil and gas industrial wastewater under natural pH conditions.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Fang Li,Nuotong Shen,Qingcheng Li,Chen Yang,Limin Zhang,Mingjin Wang
The development of microfluidic flow injection analysis (FIA) system for simultaneous and real-time detection of multiple metal ions is of great importance for environmental monitoring, food safety and industrial field. In this work, a multiplexed microfluidic chip based FIA system was fabricated for simultaneous determination of three metal ions, by using Fe(III), Mn(II) and Cu(II) as models. The multiplexed microfluidic chip based FIA system is composed of three parts, including a multi-channel FIA system for solution manipulation, a group of microfluidic chips for reagents mixing and reaction, and one fiber optic spectrometer for fast and real-time absorbance signal detection. The sample solution and chromogenic reagents were injected into the microfluidic chips to carry out specific colorimetric reactions. Fe(III), Mn(II) and Cu(II) reacts with 5-sulfosalicylic acid, formaldoxime, and bis(cyclohexanone) oxalyldihydrazone, respectively, to generate orange, ember and blue colored solution with peak absorbance at 420 nm, 450 nm, and 600 nm, respectively. The absorbance signal of the generated three channels of solution can be sequentially detected by using only one mini spectrometer. The linear detection range for Fe(III), Mn(II) and Cu(II) is 0.1–20 mg/L, 0.1–12 mg/L and 0.2–12 mg/L, respectively. The limit of detection for Fe(III), Mn(II) and Cu(II) is 0.07, 0.02 and 0.1 mg/L respectively. And the limit of quantification for Fe(III), Mn(II) and Cu(II) is 0.2, 0.07 and 0.3 mg/L, respectively. The recoveries of spiked Fe (III), Mn (II), and Cu (II) in real water samples are between 95.3 % to 106 %. Finally, the developed microfluidic chip based FIA system was successfully applied to simultaneous determination of three metal ions in environmental water samples and zinc smelting solution from zinc hydrometallurgy industry with satisfied results.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER INTERNATIONAL
·
2021
·Vol. 71
·期 2
·169-174
·
IF 2.99
Yinyan Chen,Yiban Wu,Yifan Zhu,Saiqi Tian
Rhodamine salicylaldehyde was synthesized, and its structure was determined using Fourier transform infrared spectroscopy, 1 H NMR analysis as well as electrospray ionization mass spectrometry. Then a fluorescent polyurethane foam was obtained via incorporation of the prepared rhodamine salicylaldehyde, and the fluorescence sensing behavior for Fe 3+ was systematically investigated. Results showed that the fluorescent polyurethane foam produced higher fluorescence in the presence of Fe 3+ in pure water, due to the coordination for Fe 3+ binding leading to ring-opened amide form. The limit of detection was calculated to be 1.64 × 10 −6 mol L –1 . This fluorescent polyurethane foam can also recognize Fe 3+ with good selectivity. © 2021 Society of Industrial Chemistry.
研究领域:
分析化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haonan Chen,Shiqi Tian,Zheng-Qian Liu,Jun Ma,Gang Wen
Iron oxides are widely utilized in catalytic ozonation, but their effectiveness is often limited by the slow Fe(II)/Fe(III) redox cycle. In this study, a series of metal sulfide–iron oxide composites were synthesized, all of which exhibited enhanced catalytic performance, with MoS 2 @Fe 3 O 4 showing outstanding efficiency. The catalytic system decomposes ozone (O 3 ) into hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ), with ·OH predominantly contributing to the oxidation process. The catalytic process was significantly enhanced through three key pathways: (i) metal sulfides themselves demonstrate superior ozonation catalytic performance compared to iron oxides; (ii) the presence of Mo(IV) effectively promotes the Fe(II)/Fe(III) redox cycle; and (iii) the transient superoxide radical (·O 2 − ), a crucial intermediate in ozone chain decomposition, rapidly reduces high-valence Mo(VI) to Mo(IV), thereby reinforcing the Mo redox cycle, further strengthening the Fe redox cycle, and leading to the accumulation of 1 O 2 . Notably, the efficient utilization of ·O 2 − represents a unique mechanism in the catalytic ozonation system. These findings emphasize the critical role of the Mo redox cycle in enhancing Fe redox activity to promote catalytic ozonation, providing valuable insights for the development of advanced metal sulfide–iron oxide catalysts for environmental applications.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）