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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

MOF-derived two-dimensional FeNx catalysts based on hexamethylenetetramine for efficient oxygen reduction reactions

Zichang Luo,Guoyu Zhong,Zhen Meng,Xiaobo Fu,Wenbo Liao,Shaona Zheng,Yongjun Xu,Shaojuan Luo

Although it remains a serious concern, it has become possible to create electrocatalysts that are cheap, effective, and steady for use in oxygen reduction reactions . Herein, we prepared a Fe-doped single-atom porous nitrogen-carbon catalyst by stepwise pyrolysis . The presence of FeN 4 active sites in FeNC-950–2 was confirmed by X-ray absorption spectroscopy (XAS). According to electrochemical tests, FeNC-950–2 outperformed most ORR catalysts and Pt/C in terms of ORR activity in an alkaline environment. The Zinc–air battery constructed with FeNC-950–2 delivers a peak power density of 176.4 mW cm −2 . It also possesses a cycling stability of nearly 300 h. The results demonstrate that the excellent ORR activity is due to the abundant nitrogen doping, graded porous structure, and abundant FeN 4 active sites.

CAS / MDL: 100-97-0 14024-18-1
研究领域: 材料科学 · 电化学 · 催化科学
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JOURNAL OF CATALYSIS · 2018 · IF 6.759

A study of FeNx/C catalysts for the selective oxidation of unsaturated alcohols by molecular oxygen

Jinping Zhang,Shinichi Nagamatsu,Junmou Du,Chaoli Tong,Huihuang Fang,Dehui Deng,Xi Liu,Kiyotaka Asakura,Youzhu Yuan

Transition-metal nitrides can exhibit catalytic performance comparable to that of noble metal catalysts in many reactions. However, investigations on the correlation of catalyst structure, performance, and stability are still highly demanded. Here, a series of metal nitrides were prepared and evaluated for the selective oxidation of alcohols by molecular oxygen. Among them, FeN x /C- T catalysts ( T represents the pyrolysis temperature) display above 95% selectivity to the corresponding aldehydes in the selective oxidation of unsaturated alcohols. The optimized FeN x /C-900 catalyst gives the highest TOF of 7.0 h −1 for the conversion of 5-hydroxymethylfurfural to 2,5-diformylfuran. A combination of characterizations and experiments suggests that Fe N 4 species are the main active sites. In addition, we investigate the reasons for the catalyst deactivation and provide an effective approach to regenerating the catalysts. The results indicate that the deactivated catalysts can be regenerated by heat treatment under NH 3 /N 2 after each run. Based on these studies, a plausible reaction mechanism over the FeN x /C catalysts is proposed.

研究领域: 化学 · 材料科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 25 ·期 10 ·2637-2644 · IF 5.16

Nanowire-Templated Synthesis of FeNx-Decorated Carbon Nanotubes as Highly Efficient, Universal-pH, Oxygen Reduction Reaction Catalysts

Yanqiang Li,Huiyong Huang,Siru Chen,Chao Wang,Tingli Ma

Graphical Doped to reduce : FeN x -decorated carbon nanotubes are prepared by utilizing ZnO nanowires as a sacrificial template and Fe–polydopamine (Fe–PDA) complex as metal and carbon sources (see figure). The evaporation of Zn at high temperature results in a high surface area of the carbon nanotubes, and the FeN x species contribute greatly to the oxygen reduction reaction activity of the catalyst. It is of increasing importance to develop highly active and economical oxygen reduction reaction (ORR) electrocatalysts, which have great significance for the large-scale implementation of various energy conversion systems, including metal–air batteries and fuel cells. Herein, a novel method to synthesize FeN x -decorated carbon nanotubes as a high-efficiency ORR catalyst, by utilizing ZnO nanowires as a sacrificial template and a Fe–polydopamine complex as metal and carbon sources, is reported. The obtained catalyst shows great potential for replacing Pt/C as the ORR catalyst under various pH conditions, from alkaline to acidic electrolytes. The high conductivity, large surface area of the carbon nanotube, and highly active FeN x species contributed greatly to the high performance of the catalyst. The work presented herein paves a new way for the synthesis of 1D porous nanomaterials for a broad range of energy-related applications.

CAS / MDL: 7440-06-4
研究领域: 材料科学 · 电化学 · 能源技术
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

N-doped mesoporous FeNx/carbon as ORR and OER bifunctional electrocatalyst for rechargeable zinc-air batteries

Jieting Ding,Peng Wang,Shan Ji,Hui Wang,Vladimir Linkov,Rongfang Wang

The development of low-cost bifunctional catalysts with high catalytic activity and durability for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is a critical step for successful commercialization of Zn-air batteries. In this study, N-doped mesoporous carbon containing dispersed FeN x species is prepared and tested as an ORR and OER bifunctional catalyst for this battery type. Physical-chemical characterization of the newly prepared material demonstrated that NaCl can be effective as a porous structure forming template during carbonization . Resulting mesoporous structure containing FeN x species provides significant number of ORR and OER active sites. The optimized catalyst displays higher limiting current density and more positive half-wave potential for ORR than commercial Pt/C, as well as lower overpotential for OER than RuO 2 in KOH electrolyte. Furthermore, the obtained carbon material used as an air cathode in a specially assembled rechargeable Zn-air cell demonstrates electrocatalytic performance superior to those of Pt/C and RuO 2 electrodes, which makes it a promising non-precious metal bifunctional catalyst for Zn-air batteries.

CAS / MDL: 12036-10-1
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Two-dimensional ZIF-L derived dual Fe/FeNx sites for synergistic efficient oxygen reduction in alkaline and acid media

Jun-Fei Gu,Jichao Wang,Caixia Wang,Jin Li,Cheng Chen,Ni Zhang,Xiang-Ya Xu,Somboon Chaemchuen

Fe–N–C catalysts have emerged as the most promising alternatives to commercial Pt/C catalysts for oxygen reduction reaction (ORR) due to their cost-effectiveness and favorable activity. Herein, a dual-site Fe/FeN x -NC catalyst was synthesized via a green, in situ doping strategy using two-dimensional Fe-doped ZIF-L as a nitrogen-rich precursor. The catalyst integrated Fe nanoparticles (NPs) and FeN x sites anchored on carbon nanotubes, intertwined with nitrogen-doped porous carbon nanosheets, achieving a high active site density and graphitisation. Electrochemical tests revealed that the optimized Fe/FeN x -NC-1 exhibited significant ORR activity, with a half-wave potential of 0.92 V and 0.80 V for alkaline and acidic medium, respectively. Zn-air batteries employing Fe/FeN x -NC-1 delivered a peak power density of 168 mW·cm −2 and a specific capacity of 790 mAh·g −1 , outperforming those of Pt-based catalysts. Density functional theory calculations demonstrated a reduced free energy barrier for the rate-determining step (0.48 eV) compared to single-site Fe–N 4 models (0.79 eV). The synergy between Fe NPs and FeN x optimized ORR intermediate adsorption and facilitated charge/mass transfer. This study offers valuable insights for the development of advanced energy conversion systems.

研究领域: 材料科学 · 电化学 · 催化领域
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Metal-organic frameworks-derived hollow dodecahedral carbon combined with FeNx moieties and ruthenium nanoparticles as cathode electrocatalyst for lithium oxygen batteries

Luxi Yao,Jian Lin,Shuai Li,Yuanhui Wu,Haoran Ding,Hongfei Zheng,Wanjie Xu,Te Xie,Guanghui Yue,Dongliang Peng

Owing to their high energy density, lithium-oxygen batteries (LOBs) have been drawn great attention as one of the promising electrochemical energy sources. However, the sluggish kinetics of oxygen reduction/evolution reaction (ORR/OER) hamper the widespread application of LOBs. Herein, an elaborate designed catalysts which are constructed by FeN x moieties dispersed on the network-like hollow dodecahedral carbon and then decorated with Ru nanoparticles (FeN x -HDC@Ru). Since the homogeneously dispersed FeN x moieties could promote ORR performance, and the Ru nanoparticles could facilitate OER capability, the FeN x -HDC@Ru nanocomposites used as cathode catalysts can significantly improve LOBs performance. A lower discharge and charge overpotentials of 0.15 V and 0.78 V can be detected in the first cycle, respectively, and an excellent cycle performance of 90 cycles at 200 mA g −1 and 89 cycles at 500 mA g −1 can be demonstrated. Herein, the charge transfer kinetics has been enhanced with the internal network-like hollow structure and a low impedance Li 2 O 2 /catalysts contact interface could be earned by the constructed Ru nanoparticles, these factors would lead to an efficient acceleration to the formation and decomposition of Li 2 O 2 during discharge and charge process.

CAS / MDL: 308068-56-6 14898-67-0
研究领域: 材料科学 · 电化学
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ENERGY & FUELS · 2024 · IF 5.2

FeNx/ZnSe/Fe Heterojunctions Embedded in Leafy N-Doped Carbon as Efficient Bifunctional Oxygen Electrocatalysts for Flexible Rechargeable Zn–Air Batteries

Lijuan Peng,Jiahuan Zhong,Chengkai Zhang,Yaohao Zhang,Dingsheng Yuan

Flexible quasi-solid zinc–air batteries, known for their efficiency and promising potential as an energy storage system, have found extensive applications in the fields of portable power supply, wildlife rescue, and flexible wearable devices. Herein, a FeNx/ZnSe/Fe heterojunction nanocomposite anchored on leafy nitrogen-doped carbon (FeNx/ZnSe/Fe–NC) is developed as a highly active bifunctional catalyst via one-step high-temperature selenization of Fe-doped zeolitic imidazolate frameworks 8. The formation of the heterostructure FeNx/ZnSe/Fe is conducive to accelerating electron transfer and improving the activity of the oxygen reduction reaction and oxygen evolution reaction. Moreover, FeNx/ZnSe/Fe–NC exhibits exceptional performance in liquid Zn–air batteries, comparable to the potency of industrially produced catalysts fabricated from precious metals. Notably, the gel polymer electrolyte (GPE) with a double-network structure, composed of poly(vinyl alcohol)- and polyacrylamide-modified with dimethyl sulfoxide (PVA–PAM–DMSO), exhibits significantly higher conductivity (193.5 mS cm–1) and excellent water retention (93.6%). As a result of the FeNx/ZnSe/Fe–NC catalyst and PVA–PAM–DMSO GPE, a flexible Zn–air battery with high-rate capability has been achieved, which demonstrates a high open-circuit potential of 1.51 V. This battery displays exceptional performance with excellent durability, adaptability, and adjustment capacity across a broad temperature range.

研究领域: 材料科学 · 能源存储与转换
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

A rational construction of FexOy-N-ZSM-5 catalyst with graphene structures and FeNx sites for the selective catalytic oxidation of triethylamine

Lingwu Meng,Maosheng Lin,Qirui Guo,Longzhao Zhang,Xiangyu Huang,Shule Zhang,Weihua Ma

Stabilizing metal species at the atomic level and tuning their catalytic properties is a significant challenge. Herein, an N-doped Fe x O y -N-ZSM-5 catalyst with layered and chain-like graphene structures is reported. The catalyst can selectively catalyze the oxidation of triethylamine (TEA) with an efficiency of 99.7 % at 240 °C, and maintain an N 2 yield of 97.6 % over the reaction temperature range of 240–360 °C. The results indicate that the layered graphene in the catalyst provide anchor sites for active Fe, while the abundant chain-like graphene act as connectors between ZSM-5 and the layered graphene, offering ample opportunities for TEA and its intermediates to contact the catalyst surface. This increases the number of active sites on the catalyst, thereby enhancing the catalytic performance of Fe x O y -N-ZSM-5. Notably, due to the interaction between FeO x and FeN x species, Fe x O y -N-ZSM-5 exhibits excellent thermal stability and water resistance, demonstrating promising potential for practical.

CAS / MDL: 7732-18-5 66-71-7
研究领域: 催化化学 · 材料科学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 44 ·25557-25566 · IF 10.733

Facile solution synthesis of FeNx atom clusters supported on nitrogen-enriched graphene carbon aerogels with superb electrocatalytic performance toward the oxygen reduction reaction

Min Hong,Jianhang Nie,Xiaohua Zhang,Pengfei Zhang,Qin Meng,Junlin Huang,Zhenyang Xu,Cuicui Du,Jinhua Chen

The development of non-platinum catalysts for the oxygen reduction reaction (ORR) to substitute state-of-the-art but expensive Pt catalysts is essential for the development and practical application of fuel cells. Here, combining the self-assembly and coordination interaction between graphene oxide (GO) with g-C3N4 and iron phthalocyanine (FePc), FeNx atom clusters supported on three-dimensional porous nitrogen-enriched graphene carbon aerogels were successfully prepared by one facile solution method. The obtained FeNx atom cluster catalyst (FeNx-CN/g-GEL) exhibited superb catalytic performance (E1/2 = 0.90 V) toward the ORR, which is superior to that of commercial Pt/C (E1/2 = 0.835 V) and the currently reported non-noble nanocatalysts. Additionally, the catalyst displayed a high metal utilization rate with a mass specific activity of 840 mA mgFe−1 at 0.80 V, excellent long-term stability with only a little decline after the 28 000 s test and remarkable tolerance to methanol and SCN−.

CAS / MDL: 132-16-1
研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

A secondary template strategy for synthesis of hierarchical porous carbon-hosted single-atomic FeNx and CoO towards bifunctional oxygen reduction reaction and oxygen evolution reaction

Hao Song,Xue Liu,Jie Song,Zhuang Shi,Zhen Fu,Hao Feng,Hongyan Zhuo,Wenmiao Chen,Yanli Chen

The intrinsic activity and full exposure of active sites play important roles in high performance electrocatalytic reactions. Herein, a novel "secondary template strategy" is reported, for first time, to synthesize a hierarchical porous carbon-based catalyst loaded by single-atomic FeN x and CoO nanoparticles (CoO@Fe-NC ZnO ) from well-defined ZnO-Fe-PPY precursor, in which the PPY (polypyrrole) in-situ grown on the surface of the ZnO templates followed by the outer coating of FeCl 3 . The utilization of ZnO templates involve their decomposition during the pyrolysis process, leading to the porous structures of the resulted Fe-NC ZnO . Simultaneously, the pyrolysis products of FeCl 3 (Fe/Fe 3 O 4 ) can gradually formed in the remaining parts of the decomposed ZnO, effectively preventing the collapse of the porous structures (so-called secondary template strategy). Subsequently, the introduction of CoO further enhances the intrinsic activity of the as-prepared CoO@Fe-NC ZnO for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), respectively, with an excellent half-wave potential (E 1/2 ) of 0.917 V (vs. RHE) and a low potential of 1.556 V (vs. RHE) at a current density of 10 mA cm −2 (E 10 ). Meanwhile, zinc-air batteries assembled with CoO@Fe-NC ZnO catalyst have great application potential. This work provides a pathway for the preparation of bifunctional electrocatalysts with a hierarchical porous structure.

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Controlled synthesis of FeNx-CoNx dual active sites interfaced with metallic Co nanoparticles as bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries

Yi-jin Wu,Xiao-hong Wu,Teng-xiu Tu,Peng-fang Zhang,Jun-tao Li,Yao Zhou,Ling Huang,Shi-gang Sun

Efficient bifunctional oxygen electrocatalysts are essential for high-performance rechargeable Zn-air batteries (rZABs). Herein, a porous hollow carbon nanoshell (H-Co@FeCo/N/C) in which FeN x and CoN x metal sites are atomically dispersed and interfaced intimately with metallic Co nanoparticles was derived from pyrolysis of polydopamine-coated ZnCo-ZIFs adsorbed with Fe 3+ ; the chemical interactions among different organic and metal species during the polymer-coating process was inverstigated; their role in regulating the size of the Co nanoparticles, the structure of the hollow carbon nanoshell and the formation of the FeN x -CoN x dual active sites was revealed. The H-Co@FeCo/N/C showed superior bifunctional oxygen electrocatalytic activity (Δ E  = 0.698 V) and mass activity of 6.8 A g cat. −1 at 0.9 V, outperforming the commercial Pt/C/RuO 2 catalysts or the Fe/N/C or Co/N/C counterparts. When assembled for rZABs, the H-Co@FeCo/N/C cathode displayed a long cycle life of 200 h ( E gap of about 1.0 V@10 mA cm -2 ).

研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

FeNx nanoparticles embedded in three-dimensional N-doped carbon nanofibers as efficient oxygen reduction reaction electrocatalyst for microbial fuel cells in alkaline and neutral media

Xueying Wang,Tian Yuan,Jiawen Liang,Jinxin Yang,Yangming Xie,Ling Li,Wenming Zhang

Herein, an approach is reported for the fabrication of 3D carbon nanofibers (CNFs) wrapped by carbon nanotubes (CNT) with graphitic carbon-encased FeNx nanoparticles originated from metal–organic frameworks (MOFs). It is found that Fe-FeNx@N-CNT/CNFs exhibits outstanding catalytic activity towards ORR, whose half-wave potential are 0.89 V and 0.87 V in alkaline and neutral environments, respectively, much higher than MOF-based catalysts reported so far and commercial Pt/C. When the obtained cathode catalysts are loaded in MFCs for power generation test, the experimental consequences show that the Fe-FeNx@N-CNT/CNFs cathode exhibits a supernal power density of 742.26 mW·m −2 and output current density of 3241 mA·m −2 which are comparable to Pt/C. The splendid ORR catalytic performance is mainly attributable to the three-dimensional structure of carbon nanofibers and the active sites of Fe-Nx. These result in a higher graphitization degree beneficial for electronic mobility, high specific surface area, benign mesoporous nanostructure and excellent mass transfer capability. The strategy provides a new scheme to devise and research Fe-Nx electrocatalysts with MOF-based for the conversion of clean and environment-friendly energy.

研究领域: 材料科学 · 电化学 · 能源转换 · 纳米技术 · 环境科学
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