Journal of Materials Chemistry A
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2020
·Vol. 9
·期 4
·2205-2213
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IF 11.301
Jiayi Li,Hongwei Zhang,Linqu Luo,Hao Li,Junyu He,Hongliang Zu,Lei Liu,Hao Liu,Fengyun Wang,Jianjun Song
Lithium–sulfur batteries (LSBs) have shown great potential for application in high-density energy storage systems. However, the performance of LSBs is severely hindered by the shuttle effect and the sluggish reaction kinetics of lithium polysulfides (LiPSs). Here, a Janus Fe3C/N-CNF@RGO electrode consisting of a 1D Fe3C-decorated N-doped carbon nanofibers (Fe3C/N-CNFs) side and a 2D reduced graphene oxide (RGO) side was applied as a free-standing carrier for the Li2S6 catholyte to improve the overall electrochemical performance of LSBs. The Fe3C/N-CNF layer endows the cathode with strong chemisorption abilities for LiPSs and accelerated the redox kinetics via catalyzing the conversion of LiPSs. The 2D RGO sheets serve as a microscopic physical barrier and further resist the shuttling of LiPSs. Like a hunter's trap, behind the trap lies a net. Moreover, the 3D hierarchical conductive network based on 1D N-CNF and 2D RGO sheets enables fast electron transfer. Based on the synergetic effects of chemical immobilization, catalytic abilities, and a physical barrier in a 3D conductive network, LSBs with optimal Fe3C/N-CNF@RGO electrodes exhibit robust long-term cycling stability (a decay rate of only 0.0089% per cycle at 0.5C for 300 cycles), superior rate capabilities (821.7 mA h g−1 at 2.0C), and stable cycling performance at high sulfur loading (6.29 mg cm−2). This work defines an emerging viewpoint relating to the design of novel sulfur carriers with multiple synergistic effects for application in LSBs.
研究领域:
储能
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电化学
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材料科学
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纳米材料
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电池技术
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Small
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2025
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IF 12.1
Wenli Lei,Shuang Zhang,Jiaxi Shu,Fudong Li,Zixuan Deng,Juejing Liu,Xiaofeng Guo,Yuanmeng Zhao,Changsheng Shan
Self-powered biosensors (SPBs) based on biofuel cells (BFCs) use electrical output as a sensing signal without the need of external power supplies, providing a feasible approach to constructing miniaturized implantable or portable devices. In this work, a novel nanozyme of gold nanoclusters/palladium nanocubes (AuNCs/PdNCs) heterostructure is successfully fabricated to develop an innovatively self-powered and non-enzymatic glucose sensing system. The AuNCs/PdNCs with glucose oxidase (GOD)-like activity exhibits superior electrocatalytic and non-enzymatic sensing performance toward glucose. The non-enzymatic BFCs-based SPBs system, established on the AuNCs/PdNCs (anodic catalyst) and single atomic Fe sites coupled with carbon-encapsulated Fe 3 C crystals (Fe 3 C@C-Fe SACs as a cathodic catalyst) platform, exhibits an exceptional sensitivity to glucose with 0.151 µW cm −2 m m −1 (3.4 times higher than the PdNCs), outstanding selectivity and robust stability. The outstanding performance of the BFCs-based SPBs system can be attributed to the synergistic cooperation between the PdNCs and AuNCs.
研究领域:
生物医学工程
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纳米技术
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电化学传感器
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Journal of the Taiwan Institute of Chemical Engineers
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2022
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IF 5.477
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.
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APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Binbin Feng,Qionghao Xu,Xiaoxue Wu,Chunlin Ye,Yanghe Fu,De-Li Chen,Fumin Zhang,Weidong Zhu
Owing to the competitive hydrogenation of reducible functionalized groups and the complexity of the reaction mechanism, the selective catalytic hydrogenation of nitroarene compounds to value-added amine products is challenging. Herein, we designed and prepared a series of highly efficient iron-based nanocomposites (Fe/Fe 3 C@NC–T) via direct pyrolysis of the presynthesized NH 2 –MIL–101(Fe) octahedrons under nitrogen atmosphere, wherein tiny metallic Fe/Fe 3 C nanoparticles (NPs) were homogeneously inlaid in the N-doped porous carbon matrix. Among the various derived catalysts, Fe/Fe 3 C@NC–750 exhibited the best performance, with good tolerance to several different functional groups for the catalytic transfer hydrogenation of nitroarenes to anilines using N 2 H 4 ·H 2 O as the reductant under mild conditions. This performance was also superior to those of commercial catalysts (Fe, Fe 2 O 3 , and Fe 3 C) and Fe/Fe 3 C@C–750 without N doping. The synergistic catalysis between the Fe-based NP and N dopant mainly contributed to the excellent catalytic performance of Fe/Fe 3 C@NC–750. Moreover, the mechanism study revealed that both the direct route and the condensation route were involved in this catalytic reaction system.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Sheng-Nan Zhuo,Hao Sun,Zhi-Ying Wang,Hong-Yu Ren,De-Feng Xing,Nan-Qi Ren,Bing-Feng Liu
This study, a magnetic biochar catalyst (Fe-N@MFC) with Fe 3 C and Fe 4 N was synthesized via one-step pyrolysis using waste floc as a raw material. Fe-N@MFC shows an efficient catalysis in activating peroxydisulfate (PDS) to degrade tetracycline (TC). 90.5 % of TC (5 mg/L) is removed within 60 min in the Fe-N@MFC/PDS (0.5 g/L and 1.8 mM) system with a degradation rate constant of 0.33043 min −1 . Reactive oxygen species (·OH, SO 4 ·− , 1 O 2 , and ·O 2 − ) and electron transfer are generated in the reaction system. ·OH and SO 4 ·− radicals make a major contribution to TC degradation . Variation in material structure and DFT calculations prove that the existence of Fe 3 C and Fe 4 N enhances the adsorption energy of PDS and promotes the redox reaction between PDS and Fe species (Fe 0 and Fe-N). Based on iron ion leaching, recycling experiment and application in real water, the Fe-N@MFC catalyst is found to exhibit promising potential. This work represents a progress compared to the traditional technology used for preparing Fe N C biochar catalysts and provides significant guidance for the further development of biochar in the future.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Yunpeng Liu,Xupo Liu,Cuicui Zhang,Ye Chen,Zhitao Wang,Gangya Wei,Jing Zhang,Tianfang Yang,Fengxian Zhang,Shuyan Gao
Fe-N-C catalysts have served as ideal catalysts for oxygen reduction reaction (ORR), but the strong adsorption to ORR-relevant intermediates and less utilization of Fe-N x sites endow those catalysts with inferior performance. Here, an efficient catalyst consisted of Fe-N x species and FeF 2 /Fe 3 C nanoparticles co-anchored on N, F co-doped carbon nanotubes (Fe-NF-CNTs) has been constructed through a surface modification strategy. Sodium trifluoroacetate as functional linker modified on metal-organic framework surface promotes to form abundant and accessible active sites. FeF 2 /Fe 3 C nanoparticles and hydrogen fluoride generated in pyrolysis process facilitate to construct N, F co-doped CNTs with defects and holes. N, F co-doping modifies the adsorption characteristic of Fe-N x sites, while CNTs improve the accessibility of active sites and the capability of material transport. Therefore, Fe-NF-CNTs exhibits outstanding activity (E 1/2 = 0.85 V) and stabilization (ΔE = 6 mV, 10k cycles). Impressively, Fe-NF-CNTs delivers high power density (144 and 68 mW cm –2 ) and cycle stability (300 and 60 h) in liquid and flexible Zn-air batteries, respectively. This work provides a surface modification strategy to guide the tuning of electronic structure of efficient ORR catalysts designed for renewable green energy.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Fengxian Zhang,Ye Chen,Yang Liu,Xupo Liu,Shuyan Gao
Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe 3 C nanoparticles and Fe-N X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe 3 C and Fe−N X , large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte , the optimized catalyst displays favorable ORR performance with positive onset potential ( E onset = 0.91 V), half-wave potential ( E 1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm −2 and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts .
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GREEN CHEMISTRY
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2026
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IF 9.2
Kexin Wei,Siyuan Sun,Fan Yang,Yang Sun,Junpu An,Yongfeng Li
Carbon-based free-standing catalysts can be directly used in rechargeable zinc–air batteries while maintaining a high mass transfer level, making them highly promising as electrodes to catalyze oxygen reduction reaction/evolution reaction (ORR/OER). However, the existing complex preparation processes and limited conductive pathways remain challenges for their further application. Herein, a FeS/Fe3C nanoparticle-embedded and graphene nanosheet-doped carbon catalyst with a free-standing and amorphous porous carbon structure (FeS/Fe3C@CP) is easily synthesized by a simple solute precipitation strategy, in which the well-connected porous carbon and composite graphene nanosheets construct a conductive network extending in all directions. The result of electrochemical impedance spectroscopy (EIS) highlights the lower resistance of FeS/Fe3C@CP in the electron transfer process than that of the electrode synthesized by electrostatic spinning using the same raw material, which confirms that electrons are rapidly transported in this conductive network. The obtained FeS/Fe3C@CP possesses bifunctional catalytic activity and exhibits a half-wave potential (E1/2) of 0.89 V (vs. RHE) for the ORR and a potential of 1.40 V at a current density of 10 mA cm−2 (E10) for the OER. Further, in liquid ZAB applications, the FeS/Fe3C@CP exhibits a power density of 125 mW cm−2, which is better than that of a commercial Pt/C and RuO2 mixture. DFT analysis shows that the ORR adsorption/desorption process occurring on iron atoms in the FeS/Fe3C heterojunction has a smaller energy barrier than that on single FeS or Fe3C nanoparticles. This research lays a practical foundation for the design and synthesis of free-standing carbon catalysts with rich conductive networks.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Tiantian Feng,Zhijie Cui,Pengfei Guo,Xuehong Wang,Juan Li,Xien Liu,Wenpin Wang,Zhongcheng Li
Tailoring surface composition and structures of catalysts affects their catalytic performance in hydrogen evolution reaction owing to the geometric and electronic effects. Herein, Ru nanoparticles embedded in 2D N-doped carbon nanosheets decorated with 2D Fe 3 O 4 –Fe 3 C heterostructures (Ru/Fe 3 O 4 –Fe 3 C/NC) are fabricated via pyrolysis of the mixture containing 2D-Fe 2 O 3 nanosheets, dopamine hydrochloride , RuCl 3 ·xH 2 O, and melamine . Interestingly, the good hydrogen evolution behavior is achieved on Ru/Fe 3 O 4 –Fe 3 C/NC with the high reactivity and stability. Ru/Fe 3 O 4 –Fe 3 C/NC offers an overpotential of 141 mV to realize the current density of 10 mA/cm 2 in 0.5 mol/L (M) H 2 SO 4 electrolyte. As for 1 M KOH, Ru/Fe 3 O 4 –Fe 3 C/NC promotes hydrogen evolution reactivity with 148 mV to achieve 10 mA/cm 2 . The current density slightly degrades after continuous I-t tests, verifying the good stability for Ru/Fe 3 O 4 –Fe 3 C/NC. The high reactivity might stem from high dispersion of Ru nanoparticles, enhanced conductivity due to doping N into carbon nanosheets, and heterointerfaces between Fe–O and Fe–C.
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Materials
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2020
·Vol. 13
·期 21
·4779
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IF 3.057
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
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Wei Zhang,Wei Wu,Fei Guo,Xinwei Dong
The control of morphology, structure and composition of metal–organic frameworks derived metal-nitrogen doped porous carbon (M–N–C) with high precision and accuracy is essential for the catalytic performance. While single-atom or small-sized nanometer catalysts show notable effects in catalysis, one catalyst combining the advantages of single-atom and nanometer catalysts may cultivate more benefits. Herein, we designed and successfully fabricated a series of Fe-doped ZIF–x with different morphologies (cube→truncated hexahedron→truncated octahedron) in one pot by simply adjusting the adding amount of vitamin C. After high-temperature calcination, Fe 3 C integrated with Fe single-atom planted in N -doped carbon (Fe SA /Fe NC –N–C–x) with various morphology, structure and composition could be acquired. Among them, Fe SA /Fe NC –N–C–0.75 exhibited the best catalytic performance for the transfer hydrogenation of halogenated nitrobenzenes with N 2 H 4 ·H 2 O under room temperature. Acid-leaching tests, poisoning experiments, and the density functional theory calculations showed that Fe 3 C integrated with Fe single-atom had a better catalytic effect than the separated Fe 3 C or Fe single-atom.
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Molecular Catalysis
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2020
·
IF 3.687
Li Fang,Qionghao Xu,Yanyan Qi,Xiaoxue Wu,Yanghe Fu,Qiang Xiao,Fumin Zhang,Weidong Zhu
The preparation of efficient and recyclable solid catalysts exhibiting high activity and selectivity toward the target product is a prerequisite to enhance the overall efficiency of a catalytic process. Herein, we study a series of Fe/Fe 3 C-containing nitrogen-doped porous carbon microspindles (Fe/Fe 3 C@NC–x, where x stands for the pyrolysis temperature), which are core-/shell-structured hybrids, constructed by the pyrolysis of a metal–organic framework precursor as highly selective catalysts for the oxidation of sulfides to the corresponding sulfoxides under mild conditions. The Fe/Fe 3 C@NC–x microspindles comprising Fe and Fe 3 C nanocrystals inlaid in nitrogen-doped porous carbon shells are fabricated by the direct carbonization of NH 2 –MIL–88B(Fe) polyhedra at 500 °C–800 °C and under nitrogen atmosphere. Among the various investigated catalysts, the Fe/Fe 3 C@NC–600 microspindles exhibit the best catalytic activity, higher than those exhibited by the analogue Fe/Fe 3 C@C–600 without N doping and the commercial Fe 2 O 3 , Fe 3 O 4 , and Fe 3 C used for the catalytic oxidation of sulfides owing to the synergistic contribution of the Fe 3 C sites and adequate nitrogen doping in the porous carbon support. Furthermore, the magnetically separable properties of the Fe/Fe 3 C@NC–600 microspindles enable their convenient isolation from the reaction system using an external magnet, and they can be repeatedly used for six cycles without any loss in catalytic efficiency.
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