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Journal of Water Process Engineering · 2022 · IF 7.34

Nitrogen-doped carbon material encapsulated Fe3C with dual-reaction centres to boost peroxymonosulfate activation for efficient organic pollutant removal

Xinfei Fan,Jia Yang,Na Liu,Yuanlu Xu,Yueling Yu,Chengwen Song,Yanming Liu

Peroxymonosulfate (PMS) activation based on iron-based catalyst has caught increasing attention in wastewater treatment , but is strongly impeded by the sluggish kinetics of Fe(II) recovery. In this study, nitrogen-doped carbon encapsulated Fe 3 C with dual-reaction centres coupled via C Fe channel was developed by electrospinning and Chemical Vapor Deposition (CVD) technique. The remarkable catalysis performance was conferred by the formation of C Fe short bond which linked C poor electron reaction centres from N-doped carbon frameworks and the Fe rich electron reaction centres from Fe 3 C. Fe@NC-800 achieved 100% sulfamethoxazole (SMX) degradation within 20 min, and showed excellent cycle stability after 5 cycles. The electron transfer rate between the dual-reaction region was accelerated due to short transport distance and low transmission resistance. Electrons from pollutants were compensated to Fe 3+ via C Fe bond bridges, promoting the regeneration of Fe 2+ and accelerating the efficiency of the Fe 2+ /Fe 3+ cycle. Besides, the experiments of reactive oxygen species (ROS) quenching and capture revealed the degradation pathway. Both radical and nonradical oxidation played a key role in the Fe@NC-800/PMS system. This work will offer a valuable clue on the design of multi-benefit catalysts to achieve efficient removal of pollutants in wastewater.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING SCIENCE · 2023 · IF 4.7

Metal-organic framework-derived Fe/Fe3C embedded in N-doped carbon as a highly efficient oxygen reduction catalyst for microbial fuel cells

Shuting Huang,Yanxian Geng,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jianmei Lu

Microbial fuel cells (MFCs) have become new energy approach for sustainable development. The exploitation of economic and efficient electrocatalysts for the oxygen reduction reaction (ORR) is essential for obtaining remarkable MFCs performance. Herein, metal–organic framework (MOF)-derived Fe/Fe 3 C embedded in nitrogen-doped carbon hybrids, prepared through a simple solvothermal and pyrolysis approach, are highly efficient ORR catalysts. The unique mixed dimension (1D/2D) and mesoporous structure provide abundant active sites and build transfer channels for improvement. Additionally, the presence of nitrogen doping played an important role to accelerate electron diffusion and transport. A maximum power density of 1974.75 ± 26.16 mW m −2 is earned by Fe/Fe 3 C/NC-800, and is 1.45 times of 20% Pt/C (1366.45 ± 28.65 mW m −2 ). Therefore, the Fe/Fe 3 C/NC catalyst is a prospective ORR catalyst in MFCs and in future renewable energy storage and conversion technologies.

研究领域: 材料科学 · 能源技术 · 环境科学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2018 · IF 3.235

Metal-organic framework-derived Fe3C@NC nanohybrids as highly-efficient oxygen reduction electrocatalysts in both acidic and basic media

Xinxin Yang,Xiaoli Hu,Xiuli Wang,Wei Fu,Xingquan He,Tewodros Asefa

Developing low-cost and high-performance non-precious metal catalysts (NPMCs) for oxygen reduction reaction (ORR) is of critical importance for commercialization of fuel cells. Herein, we report a NPMC consisting of Fe 3 C nanoparticles encapsulated in mesoporous N-doped carbon (N-C), which is synthesized by a simple two-step strategy comprising pyrolysis of a mixture of MIL-100(Fe) and dicyandiamide under inert atmosphere , followed by treatment of the product with acidic solution to leach removable Fe 3 C species from the material. Fe 3 C@NC-800 (the material prepared at 800 °C) exhibits superior electrocatalytic activity , high durability and excellent methanol tolerance for ORR, with catalytic performance comparable to that of commercial Pt/C in both alkaline and acidic media. Fe 3 C@NC-800's excellent catalytic activity and stability in ORR are due to its large BET surface area, its large total pore volume, its nitrogen dopants and the cooperative effects between the reactive functionalities in it as well as its excellent conductivity.

CAS / MDL: 461-58-5 31175-20-9
研究领域: 材料科学 · 电化学
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Journal of the Taiwan Institute of Chemical Engineers · 2022 · IF 5.477

Fe3C confined in N-doped carbons derived from Fe-N bearing ionic liquids for selective oxidation of styrene into benzaldehyde with molecular oxygen

Binxiong Guang,Yiwei Zhang,Yahui Xiao,Miaojun Su,Xiying Li,Yong Liu

Background It is of great significance but still a challenge in the chemical industry to develop high-efficient heterogeneous catalysts for selective oxidation of styrene into benzaldehyde with molecular oxygen. Methods Fe 3 C nanoparticles confined in N-doped carbons (Fe 3 C/NC) were prepared using Fe 3+ coordinated N-bearing ionic liquids as precursors and melamine as nitrogen source and template, followed by pyrolysis at 900 °C under N 2 atmosphere. The physicochemical properties of the as-prepared Fe 3 C/NC catalyst were analyzed by FT-IR, TG, BET, TEM, XRD, Raman and XPS, respectively, and further employed as novel heterogeneous catalyst for selective oxidation of styrene into benzaldehyde with molecular oxygen. Significant findings The results showed that the Fe 3 C nanoparticles were formed and uniformly embedded into the N-doped carbon matrix, which were confirmed to be the active sites for styrene oxidation. Moreover, the 5 % Fe 3 C/NC catalyst possessed high surface area and dominant mesoporous structure, which could expose more accessible active sites and facilitate mass transfer. As a result, the 5 % Fe 3 C/NC catalyst exhibited superior catalytic performance for styrene oxidation into benzaldehyde with the appropriate styrene conversion of 58.8 % and selectivity to benzaldehyde of 64.1 % as well as no significant activity and selectivity loss after reused at least five times.

研究领域: 催化化学 · 材料科学
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Journal of Materials Chemistry B · 2022 ·Vol. 10 ·期 17 ·3311-3319 · IF 7.571

In situ generated Fe3C embedded Fe–N-doped carbon nanozymes with enhanced oxidase mimic activity for total antioxidant capacity assessment

Rui Li,Xiaohong Qiao,Huijun Ma,Hanmei Li,Cong Li,Lihua Jin

In this work, we reported new Fe3C embedded Fe–N-doped carbon nanomaterials (Fe3C@Fe–N-CMs) generated in situ by the facile pyrolysis of Fe–Zn ZIF precursors. The resulting Fe3C@Fe–N-CMs were equipped with several desirable nanozyme features, including multiple efficient intrinsic active sites (i.e. Fe–Nx, Fe3C@C, and C–N moieties), large specific surface area and abundant mesoporous structures. As a result, these Fe3C@Fe–N-CMs displayed exceptional ability to mimic three enzymes: peroxidase, catalase and oxidase, while the Fe3C@Fe–N-CMs pyrolyzed at 800 °C, named CMs-800, showed the best enzyme-like properties. After systematically investigating the catalytic mechanism, we further explored the application of the oxidase-like properties of CMs-800 in the detection of the total antioxidant capacity (TAC) in beverages and tablets. This study not only provided a new approach to construct multifunctional carbon-based nanozymes, but also expanded the application of carbon nanozymes in the field of food quality and safety.

研究领域: 材料科学 · 生物化学 · 食品安全
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ACS Sustainable Chemistry & Engineering · 2018 · IF 6.14

Fe3C/Nitrogen-Doped Carbon Nanofibers as Highly Efficient Biocatalyst with Oxidase-Mimicking Activity for Colorimetric Sensing

Na Song,Fuqiu Ma,Yun Zhu,Sihui Chen,Ce Wang,Xiaofeng Lu

The synthesis of functional nanomaterials with unique structures and morphologies as efficient biocatalysts for sensing application has attracted tremendous interest. Herein, Fe3C nanoparticles encapsulated within nitrogen-doped carbon (Fe3C/N–C) nanofibers have been prepared through a facile electrospinning strategy and a carbonization process. The resulting Fe3C/N–C hybrid nanofibers display a superior oxidase-like performance toward the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) and other substrates, which is dependent on the formation of Fe3C nanoparticles and their crystallinity. The obtained Fe3C/N–C hybrid nanofibers-based oxidase-like catalyst shows a good long-term stability and reusability. Thanks to the unique catalytic activity for oxidase mimicking, an efficient sensing platform to sensitively determine sulfite and l-cysteine with low detection limits of 24.9 and 23.0 nM (S/N = 3), respectively, as well as excellent selectivity and anti-interference ability has been developed. This work demonstrates a versatile approach to fabricate Fe3C/N–C hybrid nanofibers as enzyme mimics with perfect catalytic efficiency, affording a facile and sensitive colorimetric approach for potential applications in biosensing and other biotechnologies.

研究领域: 材料科学 · 生物传感 · 仿生催化
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Efficient degradation of tetrabromobisphenol A by metal-organic framework-derived N-doped Fe/Fe3C@NC catalysts in sequential reduction-oxidation system

Minghui Xiang,Yueying Wang,Xinlei Ren,Zhiyuan Yang,Yujing Huang,Shiting Zhu,Long Chen,Jin Zhang,Hui Li

Tetrabromobisphenol A (TBBPA), a brominated flame retardant with environmental hazards poses challenges for degradation into less dangerous small molecule compounds using conventional single reduction or oxidation methods. In this study, N-doped Fe/Fe 3 C@NC was prepared as an efficient catalyst for TBBPA degradation in a sequential reduction–oxidation system (SROS). Nitrogen-doped carbon as support decelerated the oxidation of Fe 0 and simultaneously accelerated electron transfer within the composites. After the reduction reaction, the Fe species in Fe/Fe 3 C@NC were converted to Fe 2+ , which activated peroxymonosulfate more efficiently. Thus, the degradation rate constant ( k obs ) of TBBPA reached 0.132 min −1 , significantly higher than that of a single oxidation system (0.0464 min −1 ). In addition, the SROS generated more reactive oxygen species, especially O 2 •- and 1 O 2 , which facilitated electron transport and consequently led to the rapid degradation of TBBPA. Degradation pathways of TBBPA in a SROS were initially proposed, with TBBPA being debrominated gradually during reduction and then directly oxidized by cleaving the central carbon. TBBPA mineralization percentage in the SROS reached 86 %, which was the result of the reduction initially increased the oxidizability of the pollutant and ring-opening susceptibility. Predicting the toxicity of the intermediates revealed that the intermediate products generated by the SROS during the TBBPA degradation had lower toxicity. This study provides insights into the efficient mineralization of organic pollutants for the remediation of aquatic environments.

研究领域: 环境科学 · 催化化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

One-step growth of Ni3Fe-Fe3C heterostructures well encapsulated in NCNTs as superior self-supported bifunctional electrocatalysts for overall water splitting

Tangying Liu,Yanyan Xiang,Zhengjie Tan,Wei Hong,Zhimin He,Jilan Long,Bin Xie,Rong Li,Xinglong Gou

Ni 3 Fe-Fe 3 C heterostructures well encapsulated in N-doped carbon nanotubes (Ni 3 Fe-Fe 3 C@NCNTs) were fabricated by a facile one-step pyrolysis-growth approach. Thanks to the merits of abundant active sites, multiple heterogeneous interfaces, large electrochemical active surface area, robust structure, self-supporting configuration and remarkable synergistic effect, Ni 3 Fe-Fe 3 C@NCNTs exhibits excellent bifunctional catalytic activity and stability toward both HER and OER in alkaline media. Moreover, the Ni 3 Fe-Fe 3 C@NCNTs||Ni 3 Fe-Fe 3 C@NCNTs electrolyzer requires an ultralow voltage of 1.80 V for overall water splitting to reach a current density of 300 mA cm −2 , and it keeps stable over 300 h for continuous hydrogen generation with 100% Faradaic efficiency, surpassing Pt/C||RuO 2 electrolytic cell and showing great promise for industrial application in green hydrogen production.

研究领域: 材料科学 · 电化学
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Inorganic Chemistry Frontiers · 2020 ·Vol. 7 ·期 4 ·889-896 · IF 5.958

Synthesis of Fe3C@porous carbon nanorods via carbonizing Fe complexes for oxygen reduction reaction and Zn–air battery

Yijie Zhang,Yong Zhao,Muwei Ji,Han-ming Zhang,Minghui Zhang,Hang Zhao,Mengsi Cheng,Jiali Yu,Huichao Liu,Caizhen Zhu,Jian Xu

Fe-Based electrocatalysts on carbon substrates are considered suitable candidates for applications in Zn–air batteries due to their favorable ORR performance. Herein, unique Fe3C@N-doped porous carbon nanorods have been synthesized using a soft template method and carbonization. The material proved to have a porous hetero-structure, which is advantageous in providing effective electrocatalysis performance for oxygen reduction reaction, providing broad prospects for the development of non-precious metal electrocatalysts and metal–air batteries. This catalyst used for oxygen reduction reaction exhibits a half-wave of 0.83 V, which is close to that of the commercial Pt/C catalyst. Using the as-prepared Fe3C@N-doped porous carbon nanorods, the open circuit potential and power density of a Zn–air battery has been measured as 1.42 V and 126.4 mW cm−2, respectively, which are better than those of the commercial Pt/C. This study presents a novel strategy to prepare Fe3C@N-doped porous carbon nanorods, which can be used as highly effective oxygen reduction reaction catalysts for Zn–air batteries.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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Nanoscale · 2018 ·Vol. 10 ·期 19 ·9252-9260 · IF 7.233

3D interconnected hierarchical porous N-doped carbon constructed by flake-like nanostructure with Fe/Fe3C for efficient oxygen reduction reaction and supercapacitor

Guoning Li,Jiajun Zhang,Weisong Li,Kai Fan,Chunjian Xu

Hierarchical porous N-doped carbon with Fe/Fe3C nanoparticles, high content of N dopants (10.51 wt%), and a 3D interconnected porous architecture constructed by flake-like nanostructure was facilely prepared by carbonization of a zeolitic imidazolate framework-8 (ZIF-8) as a self-sacrificing template and potassium ferricyanide (PF) as a multifunctional iron precursor. The unique porous structure can offer a continuous pathway for electron transfer and shorten the mass transfer pathway, which contribute to both an oxygen reduction reaction (ORR) and a supercapacitor. The influence of the carbonization temperature and iron content on the performance of ORR and supercapacitor was investigated. The as-prepared composites carbonized at 800 °C (Fe-CZIF-800-10) displayed comparable ORR activity with Pt/C in alkaline media as well as excellent long-term stability, superb methanol tolerance, and appreciable onset potential in acid media. Moreover, Fe-CZIF-800-10 exhibited excellent capacity of 246 F g−1 at a current density of 0.5 A g−1 and stability in 6 M KOH. This report provides a facile approach to prepare hierarchical porous Fe/N-doped carbon as a promising electrode material for both fuel cell and supercapacitor applications.

CAS / MDL: 13746-66-2
研究领域: 材料科学 · 电化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2017 · IF 2.714

Fe/Fe3C nanoparticles loaded on Fe/N-doped graphene as an efficient heterogeneous Fenton catalyst for degradation of organic pollutants

Xiaoqin Huang,Yanli Niu,Weihua Hu

Heterogeneous Fenton catalyst with high activity and excellent durability is highly demanded for efficient removal of organic pollutants via well-known Fenton reaction. In this work Fe/Fe 3 C nanoparticles loaded on iron/nitrogen-doped graphene (Fe/Fe 3 C @ Fe/N-Graphene) were synthesized via spontaneous oxidative polymerization of dopamine (DA) on graphene oxide (GO) surface in the presence of iron (III) chloride, followed by thermal annealing. The Fenton catalytic performance of as-prepared Fe/Fe 3 C @ Fe/N-Graphene was evaluated by degrading rhodamine 6G (Rh 6G) as a model organic pollutant. It is found that as-prepared catalyst demonstrates good activity with a rate constant of 0.080   min −1 under optimal hydrogen peroxide (H 2 O 2 ) concentration and catalyst dosage. Moreover, its catalytic activity shows negligible decrease even after 13 successive cycles, exhibiting excellent catalytic durability. The possible mechanism behind the improved Fenton catalytic activity and durability was further discussed.

CAS / MDL: 7782-42-5
研究领域: 环境科学 · 材料科学
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Materials · 2020 ·Vol. 13 ·期 21 ·4779 · IF 3.057

A Facile Method for the Generation of Fe3C Nanoparticle and Fe-Nx Active Site in Carbon Matrix to Achieve Good Oxygen Reduction Reaction Electrochemical Performances

Yuzhe Wu,Yuntong Li,Conghui Yuan,Lizong Dai

Introduction of both nitrogen and transition metal elements into the carbon materials has demonstrated to be a promising strategy to construct highly active electrode materials for energy shortage. In this work, through the coordination reaction between Fe3+and 1,3,5–tris(4–aminophenyl)benzene, metallosupramolecular polymer precursors are designed for the preparation of carbon flakes co-doped with both Fe and N elements. The as-prepared carbon flakes display wrinkled edges and comprise Fe3C nanoparticle and active site of Fe–Nx. These carbon materials exhibit excellent electrocatalytic performance. Towards oxygen reduction reaction (ORR), the optimized sample has Eonsetand Ehalf-waveof 0.93 V and 0.83 V in alkaline system, respectively, which are very close to that of Pt/C. This approach may offer a new way to high performance and low-cost electrochemical catalysts.Keywords:coordination;metallosupramolecular polymer;active site;carbon materials;oxygen reduction reaction

研究领域: 材料科学 · 电化学
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