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ACS Applied Energy Materials · 2018 · IF 0

Fe/N Codoped Carbon Nanocages with Single-Atom Feature as Efficient Oxygen Reduction Reaction Electrocatalyst

Nan Jia,Qiaozhen Xu,Fengqi Zhao,Hong-Xu Gao,Jiaxin Song,Pei Chen,Zhongwei An,Xinbing Chen,Yu Chen

The electrochemical kinetics of oxygen reduction reaction (ORR) determines the energy conversion efficiency of fuel cells and metal–air batteries. Thus, developing efficient and low-cost electrocatalysts for the ORR has attracted mounting attention. Herein, a facile synthetic route is presented to achieve atomic dispersion of Fe–Nx species in N doped porous carbon nanocages, resulting in a single-atom ORR electrocatalyst. The obtained Fe/N codoped carbon nanocages exhibit a comparable half-wave potential (0.82 V) and higher limiting current density compared to the commercial Pt/C electrocatalyst. In addition, by using it as air electrode electrocatalyst, the assembled Zn–air battery device shows a specific capacity of 705 mAh g–1 at 5 mA cm–2 and a negligible voltage loss after continuous operation for 67 h. The superior performance of Fe/N codoped carbon nanocages is attributed to the porous structure and the synergetic effect of atomically dispersed Fe–Nx species and N doping.

CAS / MDL: 78-10-4
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SCIENCE OF THE TOTAL ENVIRONMENT · 2018 · IF 4.61

Novel photocatalytic system Fe-complex/TiO2 for efficient degradation of phenol and norfloxacin in water

Xinyue Wang,Yingnan Sun,Lu Yang,Qingkun Shang,Dan Wang,Tongtong Guo,Yihang Guo

Photocatalysis is one of the effective strategies to eliminate various organic pollutants in water body. In this paper we have prepared a series of new composite photocatalysts to degrade phenol and norfloxacin under visible light irradiation. They were [Fe II (dpbpy) 2 (H 2 O) 2 ]/TiO 2 , [Fe II (dpbpy)(phen) 2 ]/TiO 2 and [Fe II (dpbpy)(bpy) 2 ]/TiO 2 (dpbpy: 2,2′-bipyridine-4,4′-diphosphoric acid, phen: 1,10-phenanthroline, bpy: 2,2-bipyridyl). The results show that their photocatalytic performance and cyclic stability are much better than that of pure TiO 2 or P25. Phenol can be degraded almost completely and the active groups or substituents of norfloxacin (NOR) can be destroyed also, which greatly reduced the biological toxicity of phenol and norfloxacin in water. The possible mechanisms of improving the photocatalytic activity and stability of TiO 2 by using Fe-complex are proposed based on free radical capture test and density functional theory calculation. It is clearly that the interfacial interaction between Fe-complex and titanium dioxide directly affects the photocatalytic activity and stability of the composite photocatalyst. The conjugated structure of the complexes plays a crucial role.

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ACS Sustainable Chemistry & Engineering · 2018 · IF 6.14

Functional-Protein-Assisted Fabrication of Fe–Gallic Acid Coordination Polymer Nanonetworks for Localized Photothermal Therapy

Yaqiong Wang,Jing Zhang,Chuyu Zhang,Bingjie Li,Jiaojiao Wang,Xuejun Zhang,Dong Li,Shao-Kai Sun

Fe–polyphenols coordination polymers have emerged as a versatile theranostic nanoplatform for biological applications owing to the appealing biocompatibility of precursors from nature. Incorporating bioactive molecules with Fe–polyphenols coordination polymers is greatly significant to take full advantages of their superiorities for advanced application. Herein, we show functional-protein-assisted fabrication of Fe–gallic acid (GA) nanonetworks via a mild and facile biomineralization for photothermal therapy. Mild alkaline condition is crucial to obtain protein–Fe–GA nanonetworks with intense near-infrared absorption and their unique network structure allows reducing the leakage to the surrounding normal tissues, benefiting high photothermal therapeutic efficacy and minimal side effects. The proposed bovine serum albumin–Fe–GA nanonetworks are successfully used to eradicate tumor in vivo. In addition, this universal method can be extended to synthesize other protein-involved nanonetworks, such as human serum albumin–Fe–GA and ovalbumin–Fe–GA. More importantly, the intrinsic bioactivity of protein can be retained in the nanonetworks, and the ovalbumin–Fe–GA nanonetworks enable inducing the maturation of immune cells, showing the successful fusion of immune activity of ovalbumin into the nanonetworks. The proposed biomineralization strategy shows a bright prospect in incorporating various functional proteins, such as enzymes and antibodies, to form protein–Fe–GA nanonetworks with good biocompatibility, favorable photothermal effect, and specific biological function.

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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2018 ·Vol. 165 ·期 7 ·H348 · IF 3.662

Atomically Dispersed Fe, N Co-Doped Ordered Mesoporous Carbon for Non-Enzymatic Hydrogen Peroxide Sensing

Le Wang,Hangjia Shen,Sanshuang Gao,Xamxikamar Mamat,Guangzhi Hu

As an excellent catalyst toward hydrogen peroxide reduction, Fe-based nanomaterial like Fe-N-C configuration is promising candidate to be used for H2O2 sensing. In this work, a novel N-doped mesoporous carbon by atomically dispersed Fe-N dopant composite modified electrode (Fe/NOMC) was prepared by hard template approach and then fabricated non-enzymatic sensor was used for H2O2 determination. The morphology and property of Fe/NOMC composite were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), small angle X-ray diffraction (XRD) spectrum and nitrogen-sorption measurement, respectively. The electrochemical sensing performance of the Fe/NOMC composite modified glassy carbon electrode (GCE) was studied by cyclic voltammetry and chronoamperometry methods. An excellent performance toward hydrogen peroxide reduction was achieved in a wide range of 8–23000 μM, with limitation of detection (LOD) about 5 μM and a correlation coefficient of 0.998, as well as a short response time (2 s) and good selectivity.

CAS / MDL: 1310-58-3 78-10-4
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Canadian Journal of Chemistry · 2018 ·Vol. 96 ·期 8 · IF 1.084

Fe(NO3)3·9H2O-catalyzed aerobic oxidative deoximation of ketoximes and aldoximes under mild conditions

Yongshu Li,Nizhou Xu,Guangyao Mei,Yun Zhao,Yiyong Zhao,Jinghui Lyu,Guofu Zhang,Chengrong Ding

A mild, simple process for the effective aerobic oxidative deoximation of a wide range of ketoximes and aldoximes has been developed that utilizes Fe(NO3)3·9H2O as the single catalyst and molecular oxygen as the green oxidant. The environmentally benign protocol provides moderate to excellent yield and broad functional groups tolerance and is a valuable synthetic method for practical applications. According the relevant verification experiment, a plausible mechanism has been proposed.

CAS / MDL: 75-07-0 7782-61-8
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2018 · IF 4.841

Plasma-catalytic decomposition of ethyl acetate over LaMO3 (M = Mn, Fe, and Co) perovskite catalysts

Yuxiang Cai,Xinbo Zhu,Wenshuo Hu,Chenghang Zheng,Yang Yang,Menghan Chen,Xiang Gao

Plasma-catalytic decomposition of low concentration ethyl acetate with LaMO 3 (M   =   Co, Mn and Fe) perovskite catalyst was investigated in a coaxial dielectric barrier discharge (DBD) reactor. The combination of perovskite catalyst and plasma enhanced ethyl acetate decomposition, and the activity sequence was LaCoO 3   >   LaMnO 3   >   LaFeO 3 . Characterizations results indicated that the activation of surface oxygen species and amount of oxygen vacancies contributed to ethyl acetate decomposition remarkably. FT-IR analysis demonstrated that the employment of LaCoO3 catalyst also reduced the amount of unwanted by-products. Based on these results, reaction mechanism of ethyl acetate plasma-catalytic decomposition process was proposed.

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Inorganic Chemistry Frontiers · 2018 ·Vol. 5 ·期 9 ·2211-2217 · IF 5.106

Porous Fe–N-codoped carbon microspheres: an efficient and durable electrocatalyst for oxygen reduction reaction

Xianghong Li,Xu Sun,Xiang Ren,Dan Wu,Xuan Kuang,Hongmin Ma,Tao Yan,Qin Wei

Electrochemical oxygen reduction is a key process for many energy storage and conversion devices, and finding highly efficient, economical, and durable electrocatalysts to replace the Pt-based catalyst for the oxygen reduction reaction (ORR) is a critical obstacle. In this article, porous Fe–N-codoped materials are obtained by pyrolysis of a defined precursor of polydopamine-coated Fe3O4 as not only template but also nitrogen and iron source. In 0.1 M KOH, the as-prepared catalyst exhibited high ORR activity (onset potential of 0.949 V and half-wave potential of 0.836 V vs. RHE), with excellent electrochemical stability, durability and remarkable tolerance toward methanol. The successful synthesis of porous nanospheres provides a novel way to explore a series of mesoporous metal electrocatalysts for energy conversion.

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CERAMICS INTERNATIONAL · 2018 · IF 3.057

Hierarchical spinel NixCo1-xFe2O4 microcubes derived from Fe-based MOF for high-sensitive acetone sensor

Shumin Wu,Xianliang Li,Yan Xu,Junbiao Wu,Zhuopeng Wang,Yide Han,Xia Zhang

Hierarchically spinel Ni x Co 1- x Fe 2 O 4 (0.0 ≤  x  ≤ 0.5) microcubes were successfully prepared through a combined solvent evaporation strategy and morphology-inherited annealing treatment. By using the Fe-based metal-organic frameworks (MOFs), Fe 4 (Fe(CN) 6 ) 3 , and inorganic Ni 2+ and Co 2+ acetate salts as co-templated precursors, hierarchical Ni-doped spinel CoFe 2 O 4 architecture can be obtained, and the Ni/Co substitution ratios can be controlled systematically. The obtained cubic hierarchical Ni x Co 1- x Fe 2 O 4 , (0.0 ≤  x  ≤ 0.5) composites presented highly acetone sensing properties, among which the Ni 0.1 Co 0.9 Fe 2 O 4 composite showed the strongest response performance (with gas response ( R g / R a ) of 1.67 at 240 °C) and excellent reproducibility (for at least 14 cycles), and the proposed acetone sensing mechanism was also discussed. The presented solvent evaporation and co-templated strategy may allow precisely access to fabricating other heteroatom doped inorganic materials with intriguing morphologies, architectures, chemical compositions and tunable sensing properties.

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Analytical Methods · 2015 ·Vol. 8 ·期 6 ·1239-1248 · IF 1.821

A facile method for determining the Fe(0) content and reactivity of zero valent iron

Shaolin Li,Yangyang Ding,Wei Wang,Hong Lei

Zero valent iron (ZVI) is increasingly used in large quantities for water treatment. In large-scale application of ZVI, a common question that engineers encounter is ZVI selection or its quality assurance and quality control (QA/QC). A facile method for assessing ZVI quality is proposed and studied in this work. The method is based on the Fe(III)–Fe(0) reaction that has a fast reaction rate, a known and simple stoichiometry, and an easy-to-assay product. The method is conducted by mixing the sample (e.g., testing ZVI) with concentrated Fe(III) solution (up to 3.0 g L−1) for 3–4 hours. The metallic iron (Fe(0)) content of the sample is obtained by assaying the final increase of the total dissolved iron, and its reactivity is quantified using the observed dissolution rate constants. The method is experimentally validated using 23 iron-based materials. Studies with reference iron powder and iron oxide demonstrate that the Fe(III) solution has satisfactory specificity in selecting Fe(0). Replicate experiments and t-test evaluation show the complete dissolution of the Fe(0) content in micron-scale ZVI and the high reproducibility of the method for measuring Fe(0). The accuracy and reliability of the method are studied using 15 commercial ZVIs of known Fe(0) purity, in a series of experiments using Fe(III), Cu(II) or trichloroethylene. The experiments show that the results from the proposed method are accurate and reliable, and that the method is a strong tool more effective than conventional techniques such as X-ray diffraction and BET-N2 adsorption. This work provides an easy and facile way for the quantitative assessment of the quality of metallic iron used for environmental clean-up, especially for the quick survey of a large number of iron samples on site. The method may also serve as a QA/QC procedure for ZVI in industrial-scale production.

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CHEMICAL ENGINEERING JOURNAL · 2015 · IF 4.321

Enhanced degradation of benzene in aqueous solution by sodium percarbonate activated with chelated-Fe(II)

Xiaori Fu,Xiaogang Gu,Shuguang Lu,Minhui Xu,Zhouwei Miao,Xiang Zhang,Yacong Zhang,Yunfei Xue,Zhaofu Qiu,Qian Sui

In this study, the application of sodium percarbonate (SPC) catalyzed by various chelated-Fe(II) to stimulate the degradation of benzene in groundwater remediation was investigated. Effective oxidation of benzene was achieved in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems. The reaction mechanism for benzene degradation in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems was elucidated by free radical probe compound tests, free radical scavenger tests and electron paramagnetic resonance (EPR) analysis. And hydroxyl radical (HO ) and superoxide anion radical ( O 2 - ) were confirmed as the predominant species responsible for benzene degradation. Besides, the effects of various factors, such as the solution characteristics including the presence of anions (Cl − , HCO 3 − , SO 4 2− and NO 3 − ), natural organic materials (NOM), and the initial solution pH on benzene degradation were also evaluated. The influences caused by SO 4 2− , NO 3 − , Cl − and NOM were negligible, but HCO 3 − anion had a slightly inhibitive effect in low concentration (1   mM) and an apparently inhibitive effect in high concentration (10–100   mM). However, the additions of CIT and OA eliminated the adverse influence of HCO 3 − and ensured a high benzene degradation efficiency at wider pH range. Finally, results obtained in actual groundwater test strongly demonstrated that Fe(II)-CIT and Fe(II)-OA catalyzed SPC systems are applicable for the remediation of benzene-contaminated groundwater in practice.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2015 · IF 7.435

Excellent photo-Fenton catalysts of Fe–Co Prussian blue analogues and their reaction mechanism study

Xuning Li,Jiayi Liu,Alexandre I. Rykov,Hongxian Han,Changzi Jin,Xin Liu,Junhu Wang

Two kinds of Fe–Co Prussian blue analogues (Fe–Co PBAs) with different iron valence state, Fe 3 [Co(CN) 6 ] 2 ·12H 2 O and Fe[Co(CN) 6 ]·2H 2 O, were developed as the photo-Fenton catalysts for in-depth investigation of the heterogeneous Fenton reaction mechanism. These two catalysts showed exceptionally high efficiencies for the degradation of Rhodamine B. The efficient redox cycling of iron species in the Fe–Co PBAs photo-Fenton process was deeply explored by Mössbauer spectroscopy. The excellent photo-Fenton activities of these Fe–Co PBAs were ascribed to the existence of highly dispersed water coordinated iron sites and abundant vacancies in the metal-organic-frameworks. Singlet oxygen was identified by radical scavenger experiments and electron paramagnetic resonance spectroscopy, which plays a key role in the photo-Fenton process. Based on these comprehensive experimental results, a novel radical reaction mechanism was proposed. This work not only opens up a new avenue for the application of Fe–Co PBAs, but also gives a deeper insight into the mechanisms of heterogeneous Fenton reactions.

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CHEMICAL ENGINEERING JOURNAL · 2015 · IF 4.321

New insights into the role of organic chelating agents in Fe(II) activated persulfate processes

Donghui Han,Jinquan Wan,Yongwen Ma,Yan Wang,Ying Li,Dongya Li,Zeyu Guan

Persulfate (PS) oxidation of aniline activated by several chelating agents (CAs) mediated ferrous iron (Fe(II)) was investigated. The effects of CAs structure, CA/Fe(II) ratios and pH on PS activation were studied in batch experiments ran for 120   min. Results showed that the accessible Fe(II) in the CA–Fe(II) complex was responsible for PS activation and appropriate Fe(II) accessibility was favored for more efficient utilization of Fe(II), which could improve the PS activation. Due to the steric hindrance, the number of chelating functional groups and the molecule size of CAs determined the Fe(II) accessibility. In addition, the Fe(II) accessibility was affected by the CA/Fe(II) ratio. When the ratio was 5/1, the Fe(II) accessibility followed the sequence: citric acid   >   oxalic acid   >   tartaric acid   >   (S,S)-ethylenediamine-N,N′-disuccinic acid (EDDS), but when the ratio was lower than 3/1, the accessibility followed the sequence: oxalic acid   >   tartaric acid   >   citric acid   >   EDDS. In tartaric acid processes, as high as 91.7% PS decomposition was obtained at initial pH 9. Although the acidification of solution might contribute to the high PS decomposition, Fe(II) buffering and Fe(II) recovery possibly played more important roles. Citric acid and tartaric acid were more effective in promoting PS activation and larger PS decomposition was observed in these processes under various initial pH. However, the intense competition for radicals by tartaric acid decreased the PS efficiency for aniline removal. The results of Electron Spin Resonance (ESR) and radicals quenching experiments indicated that both SO 4 − and OH contributed to the overall oxidation performance, but OH was the dominant oxidative species.

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