JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Qiuyang Tan,Xu Chen,Houzhao Wan,Bao Zhang,Xiang Liu,Lang Li,Cong Wang,Yi Gan,Pei Liang,Yi Wang,Jun Zhang,Hanbin Wang,Ling Miao,Jianjun Jiang,Peter A. van Aken,Hao Wang
Battery-supercapacitor hybrid (BSH) devices with aqueous electrolytes receive extensive attention due to their high potential. In this study, porous carbon coated Fe 3 C nanoparticles (C/Fe 3 C) are loaded onto reduced graphene oxide (rGO) nanosheets , forming rGO@C/Fe 3 C composite structure. The rGO@C/Fe 3 C composite is prepared by in-situ carbonization of rGO/Fe-MOFs. First-principles calculation proves that the high conductivity of the Fe 3 C mainly comes from d electrons of Fe and therefore can benefit the rate capability. The optimized electrode structure of rGO@C/Fe 3 C displays high capacity of 95.3 mAh g −1 at 1 A g −1 , enhanced rate performance (retaining 66.5% at 20 A g −1 ) and outstanding cycling stability (retaining 81.5% after 5000 cycles). Furthermore, a BSH device with Na 0.5 MnO 2 cathode and rGO@C/Fe 3 C anode structure shows an ultrahigh output voltage of 2.4 V in 1 M Na 2 SO 4 electrolyte, while its output voltage in 6 M KOH electrolyte is only 1.4 V. The observed energy densities of the device in two electrolytes are 46.2 Wh kg −1 at 1.2 kW kg −1 and 28.3 Wh kg −1 at 0.7 kW kg −1 , respectively. Therefore, the successful construction of the BSH device based on Fe 3 C/rGO provides an attractive strategy for the selection of anode materials .
研究领域:
材料科学
·
能源存储与转换
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产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 6
·060526
·
IF 3.721
Fang Liu,Xiaolong Zhang,Xinquan Zhang,Minmin Liu,Qinsi Shao,Li Dong,Wei Yan,Jiujun Zhang
In this paper, a novel material of Fe3C nanoparticles encapsulated inside the bamboo-like nitrogen-doped carbon nanotubes (Fe3C@b-NCNTs) is synthesized by pyrolysis of the mixture of iron salt and melamine-formaldehyde resin/SiO2 hybrid, and explored as the electrocatalyst for air-cathode of zinc-air battery. The morphology, structure and composition of Fe3C@b-NCNTs samples obtained at three different heat-treatment temperatures (700 °C, 800 °C, and 900 °C, respectively) are characterized by SEM, TEM, HR-TEM, HAADF-STEM, XRD, XPS, Raman and BET. Through electrochemical measurements using cyclic voltammetry, linear sweep voltammetry, and chronoamperometry, the oxygen reduction reaction (ORR) performance of such catalysts are evaluated. The obtained Fe3C@b-NCNTs-800 shows high and even better activity and stability than Pt/C catalyst. The excellent ORR performance of such catalyst can be ascribed to the bamboo-like nanotube structure, the adequate nitrogen doping level, and the synergistic effect between graphitic carbon layer and Fe3C nanoparticles. It is believed that the graphitic carbon layers can prevent Fe3C nanoparticles from agglomeration and protect Fe3C nanoparticles against electrolyte corrosion, while Fe3C nanoparticles activate the neighboring graphitic carbon layers and thus boost ORR activities. A rechargeable home-made zinc-air battery (ZAB) is assembled by using this catalyst for air cathode. The high performance of the assembled ZAB suggests that this Fe3C@b-NCNTs-800 catalyst is a promising electrcatalyst for metal-air batteries.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yanan Shang,Cheng Chen,Ping Zhang,Qinyan Yue,Yanwei Li,Baoyu Gao,Xing Xu
In this work, the nitrogen-doped carbon nanotubes with encapsulated Fe 3 C nanoparticles (Fe 3 C@NCNTs) were prepared through a simple process by pyrolyzing the precursor of ferric trichloride hexahydrate and melamine composite. It was studied systematically that multiple Fe 3 C@NCNTs synthesized under 600–1000 °C activated persulfate (PS) for the degradation of sulfamethoxazole (SMX), a widely used antibiotic of sulfonamides. Raman spectrum , X-Ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS) were used to characterize the transformation of catalyst with the increase of annulling temperature. The Fe 3 C@NCNTs synthesized under 800, 900 and 1000 °C showed similar degradation ability to SMX with degradation rates of 0.650–0.893 min −1 . During catalytic process, the specific structure of Fe 3 C encapsulated NCNTs could both benefit the electron transfer and prevent the Fe 3 C dissolving in the solution. The results of quenching experiments coupling with electron paramagnetic resonance (EPR) spectra suggested the OH, SO 4 − and 1 O 2 contributed to the degradation of SMX and the singlet oxygen took effect for longer time. The degradation intermediates were mainly derived from the reactions of hydroxylation, oxidation , aniline ring opening, deamination, desulfonation, as well as bond cleavage. In terms of the density functional theory (DFT) calculations, the graphitic N exhibited the highest ΔE ads (−0.437 eV) for the PS molecule, and it was followed by the pyrrolic N (−0.304 eV), pristine graphene (−0.146 eV) and pyridine N (−0.072 eV), which means that the graphitic N is more favorable for the binding affinity with PS, forming the reactive complexes on the surface of the NCNTs catalysts to promote the nonradical oxidation.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jie Li,Hua Yin,Haoyu Luo,Yingchao Li,Xufa Rong,Zhi Dang
Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through •OH and SO 4 •– radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O 2 •– and 1 O 2 induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe 3 C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O 2 •– and 1 O 2 . The structures of Fe 3 C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O 2 •– and 1 O 2 were the primary reactive species in Fe 3 C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe 3 C were the main active sites in Fe 3 C@Fe-800 for PMS activation to generate 1 O 2 . Unlike the reported •OH and SO 4 •– mediated degradation induced by the iron-based catalyst, both O 2 •– and 1 O 2 contributed to PCB 28 degradation： nucleophilic dichlorination reaction by O 2 •- and then ring-open oxidation process by 1 O 2 . Fe 3 C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe 3 C in PMS activation to generate O 2 •- and 1 O 2 for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Hesheng Yu,Dawei Liu,Katam Srinivas,Fei Ma,Ziheng Zhang,Mengya Wang,Yu Wu,Yue Wang,Xinsheng Li,Yuanfu Chen
It is still challenging but crucial to plumb non-noble metal-based oxygen reduction reaction (ORR) catalysts with comparable or better performance than benchmark Pt/C catalysts. Herein, we proffer an unconventional core-shell-structured iron-based heterostructure electrocatalyst constructed by a Fe/Fe 3 C heterostructure nanoparticle core wrapped by a graphitic shell embedded on a conductive N-doped mesoporous graphite skeleton (Fe/Fe 3 C@NC) via facile pyrolysis of MIL-53(Fe) (MIL = Matérial Institute Lavoisier) and melamine. The Fe/Fe 3 C@NC catalyst delivers more positive half-wave potential ( E 1/2 ) of 0.86 V and a low Tafel slope of 56 mV dec −1 for ORR, outpacing the benchmark Pt/C catalyst, and it also shows remarkable long-term durability and excellent methanol tolerance. The marvelous ORR behaviors can be attributed to its distinctive morphologic structure: the heterostructure can enhance intrinsic ORR activity; the core-shell nanostructure can enhance ORR activities through unique electron transfer between iron species and their conductive carbon shells, which can also act as protective barriers to ensure long-term stability; the high-content pyridinic-N doping can be used as additional active centers; and the abundant mesopores facilitate the diffusion of electrolyte, which can further upgrade ORR activities. This study proffers a strategy to design and fabricate non-noble catalysts with well-designed nanoarchitecture and high catalytic activity.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 9
·3636-3645
·
IF 6.482
Xiaoqin Li,Taotao Gao,Qilin Liu,Yanxue Xu,Jing Li,Dan Xiao
Fiber-shaped energy storage devices (FESDs) are indispensable for developing portable and wearable electronic products. Aqueous rechargeable Ni/Fe batteries are an appropriate candidate due to the cost-effectiveness, high ionic conductivity, and great safety. However, their energy density is still far from satisfactory, hindering further practical applications. Herein, we focused on studying binder-free fibrous electrodes for high-performance FESDs based on rechargeable Ni/Fe batteries. A fast microwave-assisted synthesis method was adopted to grow active materials with a 3D conductive network which is constructed from carbon nanotubes decorated with Fe–Fe3C nanoparticles. Due to the heterogeneous structure, the active materials depicted improved electron/ion transfer, boosting the electrochemical performance of the anode. A flexible Ni/Fe battery is successfully fabricated using the aforementioned anode coupled with a NiCoO-based cathode which is synthesized by electrodeposition and a post-annealing process. Thanks to the special structure of the active materials and the fast redox reaction, the assembled flexible Ni/Fe battery achieved high electrochemical properties with a maximum volumetric specific capacity of 1.61 mA h cm−3 and energy density of 1.28 mW h cm−3. The cycling stability and mechanical flexibility were also tested, which demonstrated the prospects for practical application.
研究领域:
材料科学
·
能源存储
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 43
·21451-21459
·
IF 7.443
Jianbing Zhu,Meiling Xiao,Changpeng Liu,Junjie Ge,Jean St-Pierre,Wei Xing
Non-platinum (NP) electrocatalysts with high activity and durability for oxygen reduction reactions (ORR) are required for fuel cells and other renewable systems. To avoid trial-and-error methods and achieve the rational design and synthesis of efficient NP catalysts, in-depth knowledge of the formation/growth mechanism of nanocatalysts and the origin of active sites is highly desirable. Here, we report a new class of NP catalysts with a novel structure of Fe3C encapsulated in N-doped carbon nanotubes/C. We study the formation mechanism of the nanostructure to pave the way for controlled fabrication of high-performance NP catalysts. The encapsulation of iron into carbon occurs during the first step of CNT growth and the surface functional groups on carbon black are identified as being essential for forming CNTs. The catalyst shows ultrahigh catalytic performance in both acid and alkaline media. We also examine the structure–performance dependency. The catalytic performance is highly dependent on the nanostructure and the encapsulation of Fe3C. Fe affects the catalytic performance through electronic effects rather than by directly participating in the active sites. This result is confirmed by DFT calculations, which show an increase in the density of states and a reduction in the local work function, XPS studies, and electrochemical measurements. The likelihood of N participating in the active sites is low because the catalytic performance does not depend on pyridinic and graphitic N.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xinyu Wang,Zhuo Cai,Yifei Wang,Yifei Ma,Zhaomin Tong,Mei Wang,Jonghwan Suhr,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Previous research has fully demonstrated that the core–shell spherical structure can facilitate multiple reflection within the cavity and provide polarization relaxation at the heterogeneous interfaces. In this study, double-shell nitrogen-doped carbon-Fe 3 C-Fe (NC-Fe 3 C-Fe, referred to as CFF) nanospheres composed of hollow NC-Fe 3 C and solid NC-Fe 3 C/Fe nanospheres are synthesized in an interconnected three-dimensional structure. The double-shell is composed of nitrogen-doped carbon outer shells and Fe 3 C inner shells, derived from the carbonization of polydopamine (PDA) and controllable etching of the Fe nanotemplates in the PDA@Fe. In this strategy, the carbon shells provide dielectric loss, and the Fe 3 C and Fe contribute to magnetic loss, bringing about a magnetic-electric synergistic effect on effective electromagnetic wave absorption (EMA). By adjusting the thickness of the carbon shells and the etching time of the Fe, the CFF achieves a minimum reflection loss of −74.00 dB at a thickness of 1.91 mm, with an effective absorption bandwidth of 5.04 GHz. In addition, by the radar cross-section (RCS) scattering simulation, the RCS value at a scattering angle of 0° decreased by 32.06 dBm 2 , confirming an excellent EMA capability in practical far-field applications. This study provides an effective strategy for the application of core–shell and double-shell structures in the EMA materials.
研究领域:
材料科学
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电磁学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yang Yuan,Youzhen Liu,Chenhui Li,Shi Feng,Qingquan Liu,Jia Huo
The electrocatalytic oxygen reduction reaction (ORR) plays an important role in renewable energy storage and conversion systems such as polymer electrolyte membrane fuel cells. However, design of high-performance cathode electrocatalysts is still required to speed up the sluggish kinetics of ORR. In this work, we develop a facile strategy to synthesize hierarchically porous N-doped carbon nanosheet networks with ultrafine encapsulated Fe 3 C and Fe-N x for ORR by consideration of thermodynamic (intrinsic and support effect) and kinetic (diffusion effect) parameters. The synthetic process is straightforward and sustainable and the hierarchically porous materials can be synthesized directly starting from raw materials and without any additional template. The as-designed catalyst exhibits excellent ORR catalytic performance in both acidic and basic media with much positive half-wave potential and good stability, which is comparable to commercial Pt/C. The excellent ORR performance may result from highly active Fe-N x sites and ultrafine encapsulated Fe 3 C, and the hierarchically porous nanosheet structure for accelerating mass diffusion and increasing exposure of the active site. This work provides a facile strategy for rational design and synthesis of highly active, hierarchically porous non-precious metal electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Zhaoxia Cao,Jingyi Jia,Shengnan Chen,Haohan Li,Min Sang,Mingguo Yang,Xiaoxu Wang,Shuting Yang
A low-cost in situ formed Fe2O3–Fe3C heterostructure highly dispersed in carbon nanofiber was delicately designed via a facile one-pot electrospinning method. The intense anchoring (by Fe2O3) and rapid electron transfer (by Fe3C) for lithium polysulfides transformation can be simultaneously achieved on the Fe2O3–Fe3C heterostructure interface, thus preventing the amassment of lithium polysulfides benefiting from its excellent interfacial contact and improving sulfur utilization. Experimental characterizations and DFT calculations confirmed the restrained polysulfides shuttle and enhanced redox kinetics. Therefore, the battery containing optimal Fe2O3–Fe3C heterostructure delivered a high capacity of 776.2 mA h g–1 after 300 cycles at 1 C at a low fading rate of 0.037% per cycle. Even at a high sulfur loading of 3.5 and 4.5 mg cm–2, high capacities of 773.6 and 533.6 mA h g–1 at 0.5 C can be achieved with capacity retentions of 91.7 and 94.2%, respectively. This distinctive heterostructure proposes an effective design of high-performance lithium–sulfur batteries contributing to the excellent electrochemical performance, which can synergize the virtues of effectively adsorptive metal oxides and appealing conductive metal carbides.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jinli Qiu,Yao Feng,Zhiqin Luo,Xinying Chu,Xiaoxue Pan,Fuqiang Liu
Heterogeneous Electro-Fenton (HEF) technology, which requires only oxygen and electric energy, holds significant potential for organic wastewater treatment due to its high efficiency. In this study, an iron-carbon composite cathode catalyst (Fe 3 C/BC) featuring highly dispersed Fe 3 C active sites on biochar (BC) was designed and synthesized to degrade nitenpyram (NTP), a representative neonicotinoid pesticide. The optimized Fe 3 C/BC-HEF system exhibited remarkable catalytic activity for NTP degradation, along with strong pH tolerance (3.0–9.0) and adaptability to various water matrices. This excellent performance can be attributed not only to its enhanced H 2 O 2 generation capability but also to the obviously faster H 2 O 2 activation efficiency to produce reactive oxygen species (ROS) for NTP degradation. Reactive species quenching experiments and electron paramagnetic resonance (EPR) spectroscopy confirmed that singlet oxygen (¹O 2 ) was the dominant reactive species responsible for NTP degradation. Furthermore, combined with HPLC-MS/MS analysis and Fukui index calculation, the intermediate products and degradation pathway of NTP were verified. The excellent reusability and stability of the cathode could be due to the protective role of BC, which minimized direct contact between Fe₃C active sites and the reaction solution, and thus reducing Fe 3 C corrosion during the HEF process. This study offers important insights into the design of superior metal-carbon hybrid cathode for electrochemical water remediation technologies.
研究领域:
环境科学
·
电化学工程
·
农药污染治理
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产品关联
DOI
高影响因子
ACS Biomaterials Science & Engineering
·
2019
·
IF 4.511
Sihui Chen,Yixian Wang,Mengxiao Zhong,Dahai Yu,Ce Wang,Xiaofeng Lu
In the past decade, nanomaterials-based artificial enzymes have emerged as a hot spot in the field of catalysis. However, it is a significant challenge to fabricate functional nanomaterials for multiple-enzyme mimetic activity. In this work, we have presented an efficient catalytic platform to mimic peroxidase, oxidase, and catalase-like activity by Fe3C decorated carbon nanofibers (Fe3C/C NFs). First, polyacrylonitrile nanofibers (PAN NFs) are prepared via an electrospinning technique. Next, an Fe(III)-tannic acid (TA) complex is formed on the surface of PAN NFs through a wet chemical reaction. Finally, Fe3C/C NFs are obtained from the carbonization of the PAN/Fe(III)-TA complex nanofibers. The prepared Fe3C/C NFs show an excellent triple-enzyme mimetic property including peroxidase-like, oxidase-like, and catalase-like activity, which is investigated thoroughly by the colorimetric experiment of the 3,3′,5,5′-tetramethyl benzidine oxidation and the degradation of H2O2. Thanks to the superior catalytic performance of Fe3C/C NFs for oxidase mimicking, a facile and colorimetric way to determine glutathione with a high sensitivity and favorable selectivity has been achieved. This work provides an efficient platform for multiple-enzyme mimicking, which may expand their promising applications in biosensing, biomedicine, and environmental technology.
研究领域:
材料科学
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生物医学
·
环境科学
✓ 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）