GEOCHIMICA ET COSMOCHIMICA ACTA
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2018
·
IF 4.69
Tongxu Liu,Dandan Chen,Xiaobo Luo,Xiaomin Li,Fangbai Li
Redox reactions between iron and nitrogen drive the global biogeochemical cycles of these two elements and, concomitantly, change the fate of nutrients in and the mineralogy of the cycles. The microbially mediated NO 3 − -reducing Fe(II) oxidation process (NRFO) plays a key role in Fe/N interactions under neutral-anoxic conditions. Microbially mediated NRFO was considered a biological process, yet recently it has been documented that chemical mechanisms are also at play. However, the relative contributions of biological processes and chemical processes to Fe(II) oxidation remain largely unquantified owing to the co-occurrence of the reactions. Herein, the kinetics and secondary minerals of microbially mediated NRFO by Pseudogulbenkiania sp. strain 2002 and Acidovorax sp. strain BoFeN1 were investigated with acetate as electron donor unless otherwise stated. The results of Cells + NO 3 − suggested the two strains could biologically reduce NO 3 − to NO 3 − /NO x /N 2 O/N 2 and concomitantly oxidize acetate and result in cell growth. Fe(II) oxidation and NO 3 − reduction occurred simultaneously in the presence of Fe(II) (Cells + Fe(II) + NO 3 − ). For strain BoFeN1, the presence of Fe(II) slightly enhanced the NO 3 − reduction, acetate consumption, and cell growth, all of which were substantially retarded by Fe(II) for strain 2002. When compared with the microbial nitrite reduction, the relatively higher rate of chemical reaction between NO 2 − and dissolved Fe(II) confirmed the occurrence of chemodenitrification in the microbially mediated NRFO processes. After 5 days’ incubation, no green rust was observed, and lepidocrocite , goethite , and magnetite were observed with the Cells + Fe(II) + NO 3 − treatment, but only goethite was found with the Fe(II) + NO 2 − . The spectra for the EPSs + Fe(II) treatment suggested that the oxidized c -Cyts in the EPSs could oxidize Fe(II), which show the theoretical capability of taking electrons from Fe(II) into the cells via c -Cyts. A brief model was established by combining the verified reactions of (1) biological reduction of NO 3 − to NO 2 − /NO x /N 2 O/N 2 , (2) Fe(II) oxidation by NO 2 − , and (3) Fe(II) oxidation by c -Cyts in EPSs. Based on the model, the rate constant of Fe(II) oxidation by c -Cyts in EPSs was derived. For nitrite reduction, the relative contribution of biological processes to the nitrite reduction was higher than that of chemodenitrification. For Fe(II) oxidation, the relative contribution of the chemical process via nitrite to Fe(II) oxidation was higher than that of biological processes. These findings provide a quantitative interpretation of the chemodenitrification and biological reactions in the microbially mediated NRFO processes, which could assist the mechanistic understanding of the global biogeochemical cycles of iron and nitrogen in subsurface environments.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 32
·12186-12192
·
IF 4.052
Jiang-Yan Xue,Fei-Long Li,Zhong-Yin Zhao,Cong Li,Chun-Yan Ni,Hong-Wei Gu,Pierre Braunstein,Xiao-Qing Huang,Jian-Ping Lang
The development of bifunctional non-noble metal electrocatalysts demonstrating high activity and stability for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of great significance for renewable and clean energy. In this work, we report hierarchically structured integrated Fe–MoS2/Ni3S2/NF (NF = nickel foam) materials prepared by a facile in situ solvothermal method, and among them, the Fe-doped MoS2 was assembled into spine-like nanorods. The optimized electrocatalyst (denoted as Fe–MoS2/Ni3S2/NF-2) demonstrated excellent activity and durability for performing the HER and OER in an alkaline electrolyte (pH = 14) with low overpotentials of 130.6 mV and 256 mV (vs. RHE) at a current density of 10 mA cm−2, as well as no significant loss in catalytic performance even after 2000 cyclic voltammetry (CV) cycles. An outstanding durability of 180 h could be achieved for OER. The overall water splitting made up of the two-electrode system with Fe–MoS2/Ni3S2/NF-2 as both the anode and the cathode required a voltage of only 1.61 V to drive a current density of 10 mA cm−2 along with an outstanding long-term stability of 20 h, displaying its great potential for application in water splitting. The effective construction of multi-component synergistic structures shows a good pathway for high-performance electrocatalysis and energy storage.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Xiong Song,Suqing Wang,Guoping Chen,Tuo Gao,Yue Bao,Liang-Xin Ding,Haihui Wang
A novel lightweight, multi-functional layer comprised of 1D porous Fe-embedded nitrogen-doped carbon nanofibers (Fe-N-C) and 2D graphene sheets is introduced to modify a commercial polypropylene (PP) separator for use in lithium-sulfur batteries. Benefiting from the high electrical conductivity and strong lithium polysulfide (LiPS) chemical adsorption ability of Fe-N-C, the porous intercalation-structured modified layer exhibits excellent ability to suppress LiPS shuttling while maintaining high lithium-ion transport, and the modified layer functions as a highly conductive upper current collector to reutilize active sulfur species. The cell assembled with the modified multifunctional separator shows a high rate capability and excellent cycling stability, exhibiting a capacity of 847.9 mAh g −1 at 2 C and a low degradation rate of 0.053% per cycle over 500 cycles at 0.5 C.
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APPLIED CLAY SCIENCE
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2012
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IF 2.474
Zhujian Huang,Pingxiao Wu,Xing Zhang,Xiaorong Wang,Nengwu Zhu,Jinhua Wu,Ping Li
In this study, intercalation of Fe(III) complexes [Fe(Ox) 3 ] 3− and [Fe(Cit) 2 ] 3− in Mg 2 Al layered double hydroxides (LDHs) had been carried out by different routes: direct self-assembly, reconstruction and anion exchange. The result of XRD indicated that these two kinds of Fe(III) complexes intercalated LDHs (LDHs/Fe-complexes) could be successfully synthesized by anion exchange obtaining two well crystallized LDHs both with a large basal spacing. The chemical environment of iron ion in the intercalated Fe complexes was determined by FTIR , XPS and XAFS, the results of which concertedly proved that the intercalated Fe complexes were well preserved in the interlayer of LDHs. The arrangement of the Fe(III) complexes anions in the galleries of LDHs was studied by one-dimensional electron density projection. The results showed that the [Fe(Ox) 3 ] 3− anions were probably accommodated in the gallery of LDHs as an interdigitated bilayer arrangement, and the [Fe(Cit) 2 ] 3− were perpendicularly arranged against the LDHs sheets. Through the research, it is proved that the obtained LDHs/Fe-complexes markedly enhanced the UV–vis absorption ability of Fe complexes.
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CHEMOSPHERE
·
2024
·
IF 8.1
Yunzhan Ying,Shikun Liang,Fayang Zhang,Xiangwei Xu,Chenbo Qian,Long Jiang,Jing Zhou,Yulong Wan,Lie Wang,Yuyuan Yao
The harmful impact of organic pollutants on aquatic ecosystems underscores the pressing need for effective remediation. While activating peroxymonosulfate (PMS) with Fe catalyst offers a promising approach for eliminating these pollutants, its widespread use is hindered by the sluggish regeneration of Fe 2+ from Fe 3+ . Here, this study demonstrates for the first time that combining an Fe catalyst with Mo 2 C (Fe-Mo 2 C) enhances the Fe³⁺/Fe 2 ⁺ cycle, thereby improving PMS activation. The Fe-Mo 2 C/PMS system achieved near-complete degradation of carbamazepine (CBZ) within only 8 minutes, with an impressive observed rate constant ( k obs ) of up to 0.624 min -1 , about 15 times greater than that of Fe-C catalyst. It also exhibits the capability to degrade a broad range of common antibiotics, phenols, and dye-like organic compounds. Through electron paramagnetic resonance (EPR) analysis and quenching experiments, it was verified that hydroxyl radicals (·OH), sulfate radicals (SO 4 ·- ), singlet oxygen ( 1 O 2 ), and superoxide radicals (·O 2 - ) species during the reaction, with the former three serving as the primary active species. These findings offer a hopeful avenue for the systematic development and enhancement of catalysts specifically designed to efficiently remediate organic pollutants in wastewater.
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RSC Advances
·
2015
·Vol. 5
·期 83
·68200-68208
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IF 3.84
Yuezhong Wen,Ying Liang,Chensi Shen,Hongkai Wang,Dongmei Fu,Hongyu Wang
A green efficient strategy for the combination of biodegradation and adsorption methods is urgently desired nowadays to degrade dyes in an economical and effective way. In this study, a kind of novel, environmentally friendly and efficient hybrid for the fungus and chitosan–Fe membrane has been fabricated by the alginate approach. Myrothecium verrucaria I-5 and C-1, deuteromycete fungi capable of producing laccase to degrade dyes, have been used. It is found that the chitosan–Fe membrane can excellently immobilize the fungi mycelia and enzyme, and after the immobilization, the fungi and enzyme still maintain a high activity after the dye decolorization. Also, the immobilized fungi membranes have been proved to have a high efficiency for dye decolorization. Simultaneously, the decolorization ability of the crude enzymes, which are extracted from I-5 and C-1 medium, and the decolorization ability of chitosan–Fe membrane are also investigated, respectively. The results demonstrate that the dyes can be removed by the fungi and the membrane synergistically. In addition, different kinds of dyes are successfully removed with chitosan–Fe immobilized fungi membranes. These results demonstrate that dyes are first adsorbed on the chitosan–Fe membrane, decreasing the toxicity to the fungus, and then bio-degraded by the laccase produced from the fungi on the membrane.
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ACS Catalysis
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2015
·
IF 9.312
Dengke Wang,Mengtao Wang,Zhaohui Li
Phenol is one of the most important chemicals in industry. One-step selective benzene hydroxylation is an attractive yet challenging method for phenol production, especially when such a reaction can be driven by solar energy. Herein, we reported that a highly selective benzene hydroxylation to phenol can be achieved over two Fe-based metal–organic frameworks [MIL-100(Fe) and MIL-68(Fe)] under visible light irradiations using hydrogen peroxide (H2O2) as an oxidant. An optimal benzene conversion of 30.6% was achieved with a H2O2:benzene ratio of 3:4 over MIL-100(Fe) after 24 h irradiations. ESR results and the kinetic studies suggested that a successful coupling of the photocatalysis of Fe–O clusters in Fe-based metal–organic frameworks (MOFs) with a Fenton-like route is involved in this benzene hydroxylation process. The comparison of the reaction over MIL-100(Fe) and MIL-68(Fe) reveals that the structure of MOFs significantly influences the photocatalytic efficiency. Because the composition and the structure of MOFs are highly tunable, this study highlights the great potential of using Fe-based MOFs for photocatalytic benzene hydroxylation to form phenol, which may result in an economical, sustainable, and thus green process for phenol production.
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JOURNAL OF ADVANCED OXIDATION TECHNOLOGIES
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2016
·Vol. 19
·期 2
·358-365
·
IF 0.738
Yanfang Liu,Guixia Li,Zhili Zhang,Xiang Gao,Jianrui Niu,Junna Zhao,Zaixing Li
γ-Al 2 O 3 supported Manganese and Ferric oxide (Mn-Fe/Al 2 O 3 ) were synthesized and used as catalyst for ozonation of bisphenol A (BPA) in aqueous solution. It was conducted in a semi-batch reactor under different operational conditions, i.e., varying initial pH, ozone flow rate, initial BPA concentration and catalyst dosage. The results indicated that the presence of Mn-Fe/Al 2 O 3 lead to a great enhancement in ozonation of BPA. Using 5 g/L Mn-Fe/Al 2 O 3 evaluated BPA (50 mg/L) removal efficiency up to 84.1% under particular reaction conditions, while that of the single ozonation process was 48.5%. The influence of tert-butanol demonstrated that initiation of hydroxyl radicals was involved and plays an important role in catalytic ozonation. The decrement of solution pH in catalytic ozonation was much higher than that in ozone alone, indicating much small molecule acids produced in catalytic ozonation process. The repeated use the Mn-Fe/Al 2 O 3 proved that it had a good reusability and stability.
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CHEMICAL ENGINEERING JOURNAL
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2016
·
IF 5.31
Yunfei Xue,Xiaogang Gu,Shuguang Lu,Zhouwei Miao,Mark L. Brusseau,Minhui Xu,Xiaori Fu,Xiang Zhang,Zhaofu Qiu,Qian Sui
The ability of Fe(II)-activated calcium peroxide (CaO 2 ) to remove benzene is examined with a series of batch experiments. The results showed that benzene concentrations were reduced by 20–100% within 30 min. The magnitude of removal was dependent on the CaO 2 /Fe(II)/Benzene molar ratio, with much greater destruction observed for ratios of 4/4/1 or greater. An empirical equation was developed to quantify the destruction rate dependence on reagent composition. The presence of oxidative hydroxyl radicals (HO ) and reductive radicals (primarily O 2 − ) was identified by probe compound testing and electron paramagnetic resonance (EPR) tests. The results of the EPR tests indicated that the application of CaO 2 /Fe(II) enabled the radical intensity to remain steady for a relatively long time. The effect of initial solution pH was also investigated, and CaO 2 /Fe(II) enabled benzene removal over a wide pH range of 3.0–9.0. The results of radical scavenging tests showed that benzene removal occurred primarily by HO oxidation in the CaO 2 /Fe(II) system, although reductive radicals also contributed. The intermediates in benzene destruction were identified to be phenol and biphenyl. The results indicate that Fe(II)-activated CaO 2 is a feasible approach for treatment of benzene in contaminated groundwater remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Xiaori Fu,Xiaogang Gu,Shuguang Lu,Virender K. Sharma,Mark L. Brusseau,Yunfei Xue,Muhammad Danish,George Y. Fu,Zhaofu Qiu,Qian Sui
Complete degradation of benzene by the Fe(III)-activated sodium percarbonate (SPC) system is demonstrated. Removal of benzene at 1.0 mM was seen within 160 min, depending on the molar ratios of SPC to Fe(III). A mechanism of benzene degradation was elaborated by free-radical probe-compound tests, free-radical scavengers tests, electron paramagnetic resonance (EPR) analysis, and determination of Fe(II) and H 2 O 2 concentrations. The degradation products were also identified using gas chromatography-mass spectrometry method. The hydroxyl radical (HO ) was the leading species in charge of benzene degradation. The formation of HO was strongly dependent on the generation of the organic compound radical (R ) and superoxide anion radical (O 2 − ). Benzene degradation products included hydroxylated derivatives of benzene (phenol, hydroquinone, benzoquinone, and catechol) and aliphatic acids (oxalic and fumaric acids). The proposed degradation pathways are consistent with radical formation and identified products. The investigation of selected matrix constituents showed that the Cl − and HCO 3 − had inhibitory effects on benzene degradation. Natural organic matter (NOM) had accelerating influence in degrading benzene. The developed system was tested with groundwater samples and it was found that the Fe(III)-activated SPC has a great potential in effective remediation of benzene-contaminated groundwater while more further studies should be done for its practical application in the future because of the complex subsurface environment.
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JOURNAL OF POWER SOURCES
·
2016
·
IF 6.333
Yanli Niu,Xiaoqin Huang,Weihua Hu
Oxygen reduction reaction (ORR) electrocatalysts with high activity, low cost and good durability are crucial to promote the large-scale practical application of fuel cells. Particularly, iron carbide (Fe 3 C) supported on nitrogen-doped carbon has recently demonstrated compelling promise for ORR electrocatalysis . In this paper, we report the facile synthesis of mesoporous Fe/N-doped graphene with encapsulated Fe 3 C nanoparticles (Fe 3 C@Fe/N-graphene) and its superior ORR catalytic activity . This hybrid material was synthesized by the spontaneous oxidative polymerization of dopamine on graphene oxide (GO) sheets in the presence of iron ion , followed by thermal annealing in Argon (Ar) atmosphere. As-prepared material shows high ORR catalytic activity with overwhelming four-electron reduction pathway, long-term durability and high methanol tolerance in alkaline media . This work reports a facile method to synthesize promising ORR electrocatalysis with multiple components and hierarchical architecture, and may offer valuable insight into the underlying mechanism of Fe 3 C-boosted ORR activity of Fe/N doped carbon.
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JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2016
·Vol. 47
·期 3
·361-367
·
IF 2.223
Xiao Mingshu,Zhang Zhonghui,Tian Yanping,Miao Yuqing,Wang Jiahai
Abstract In this work, the synthesis of Co–Fe–Se ultrathin nanosheet-fabricated microspheres was reported for the first time as electrocatalysts toward hydrogen evolution reaction (HER). The Co–Fe–Se ternary compounds exhibited high electrocatalytic activity of HER with low onset potential in acid media due to the high specific surface area of Co–Fe–Se ultrathin nanosheet-fabricated microspheres. The presence of multiwall carbon nanotubes improved the immobilization effect of Co–Fe–Se catalysts and electron transfer between catalysts and electrode surface, leading to the improved stability and HER electrocatalysis. The non-noble metal-based ternary compounds of Co–Fe–Se obtained from earth-abundant elements may enlighten a new way of exploring cost-effective catalysts for HER to develop hydrogen energy. Graphical Abstract
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危险品化学品经营许可证（带存储）