NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 45
·20762-20769
·
IF 3.3
Yunxiao Zhang,Wenhua Xiao,Jingqiang Zhang,Tiantian Hu,Shanxia Hu,Minjie Zhou,Zhaohui Hou,Yu Liu,Binhong He
The currently leading oxygen reduction reaction (ORR) catalysts are non-precious metal electrocatalysts. However, porous structure engineering and accessibility of Fe–N–C sites still remain a huge challenge. Here, we developed hierarchically porous Fe–N–C catalysts for cathodes of Zn–air batteries using a gas diffusion strategy, which has dense active Fe–Nx moieties. The Fe-NCNF-120 catalyst provided high kinetic current density and mass activity towards the ORR, as well as a more positive initial potential and half-wave potential (Eonset = 1.00 V, E1/2 = 0.90 V). According to experiments, the outstanding ORR activity can be attributed to the organized micro- and mesoporous structure, enhanced intrinsic activity of dense and accessible active sites Fe–Nx, and the facilitated mass and electron transport by 3D interconnected pores. As the cathode for Zn–air batteries, Fe-NCNF-120 demonstrated high power density, a high open-circuit voltage, and excellent stability. The combination of inherent activity with dense and accessible spots in this work opens up new possibilities for the design and synthesis of effective electrocatalysts for energy storage and conversion.
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DOI
高影响因子
CARBON
·
2025
·
IF 11.6
Hao Lu,Xianchu Wang,Chenyu Wang,Qihang Wang,Jingjing Xie,Weiming Wang,Zhengyi Fu,Zhaoyong Zou
Zeolitic Imidazolate Frameworks (ZIF-8) has emerged as promising candidate for alleviating the aggregation of Fe 3 N-catalysts, exhibiting significantly improved oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for rechargeable zinc-air batteries. To further improve the catalytic performance, it is crucial to fabricate ZIF-8 with hierarchically porous structures, which remains challenging due to the rapid crystallization kinetics and the weak interactions. Inspired by biological porous materials, we developed a novel method using 1,3,5-trimethylbenzene TMB as a mediating molecule to dynamically regulate the organic-inorganic interface between templates and ZIF-8 precursors, achieving the micro-meso-macropores of ZIF-8, which synergistically enhances mass transport and active site accessibility. Additionally, TMB preserves the weakly alkaline environment required for ZIFs’ structural integrity by leveraging its hydrophobic co-solvent effect. The as-synthesized Fe 3 N-HPZIF-8 catalyst integrates Fe 3 N active sites, hierarchically porous structures, and pyrrolic-N dopants, resulting in the exceptional bifunctional activity in alkaline media (ΔE = 0.619 V), exceeding most benchmark catalysts. When integrated into zinc-air batteries, a peak power density of 205.2 mW cm -2 is achieved. This work presents a generalizable synthetic approach for high-performance metal-air battery catalysts.
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高影响因子
LANGMUIR
·
2026
·
IF 4.4
Yankun Wei,Dan Wang,Jinxiang Chou,Ruopeng Li,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Abstract Developing Fe–N–C electrocatalysts with high active site utilization remains a key challenge for the oxygen reduction reaction (ORR), primarily because of the limited accessibility of Fe-Nx sites. Herein, a hierarchically porous Fe–N–C (HP-Fe–N–C) catalyst is constructed via a ZnO-templated strategy combined with urea-assisted secondary pyrolysis, enabling the simultaneous regulation of the pore structure and Fe-Nx site density. The ZnO template governs the formation of mesoporous architectures, and concurrently, the pyrolysis of urea releases gaseous species that facilitate the enlargement and interconnection of mesoporous channels. Notably, the balanced micromesoporous structure derived from the ZnO template facilitates efficient mass transport and enhances site accessibility, while urea regulates the nitrogen species to promote the formation of dense Fe-Nx moieties. As a result, the HP-Fe–N–C catalyst delivers a high half-wave potential of 0.90 V, along with near four-electron selectivity and excellent durability. The Zn-air battery assembled with the HP-Fe–N–C cathode achieves an open-circuit voltage of 1.52 V, a specific capacity of 745.6 mAh g–1, and favorable charge–discharge stability exceeding 800 h. This work reveals the balance between hierarchical porosity and active site density in the Fe–N–C catalyst for the high-performance ORR.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Aojie Li,Qiao Jiang,Tianyi Suo,Liang Chen,Hong Yin,Junlin Huang,Wen-Yuan Xu,Yuan Li,Binhong He,Wei Wang
Non-noble metal single-atom catalysts with high catalytic activity have garnered considerable attention from researchers in recent years. Yet, their synthesis is affected by various factors, making process optimization a challenging and systematic task. In this study, single-atom Fe–N–C porous hollow microspheres were successfully synthesized via ultrasonic spray pyrolysis, with machine learning employed to optimize the fabrication process. Machine learning models, trained on pre-experimental data, identified the key factors influencing material structure and oxygen reduction reaction (ORR) performance. The resulting Fe–N–C (600–900) material demonstrated excellent ORR activity with a half-wave potential of 0.865 V, along with high stability and methanol tolerance. When applied to traditional liquid zinc–air batteries (ZABs), it achieved an open-circuit voltage of 1.56 V and a maximum power density of 313.4 mW cm–2, with a discharge capacity of 806.5 mAh gZn–1 at 10 mA cm–2, outperforming commercial noble metal catalysts. This work offers valuable insights into the application of machine learning for optimizing ORR catalysts and designing high-performance materials for energy conversion devices.
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DOI
PubMed
高影响因子
CARBON
·
2025
·
IF 11.6
Qunying Wang,Jie Guo,Jiaqing Zhao,Wei Wang,Shan Lu,Junmao Qie,Mark H. Rümmeli,Ruizhi Yang
Due to the high energy conversion efficiency and environmental friendliness, proton exchange membrane fuel cells (PEMFCs) have attracted significant attentions for advancing clean energy technologies. However, the sluggish kinetics of the cathodic oxygen reduction reaction (ORR) severely limits the performance of PEMFCs. The high cost and poor durability of platinum-based electrocatalysts necessitate the development of alternative low-cost transition metal and N co-doped carbon (TM-N-C) catalysts. Nevertheless, the ORR activity of TM-N-C is limited by the low density of exposed active sites TM-N x on carbon. Herein, a combined high internal phase emulsion (HIPE) soft template and ZnO hard template is developed to fabricate porous Fe and N co-doped carbon (HP-Fe-N/C) catalyst. This coupled soft-hard template approach enables the construction of a hierarchical porous structure with high exposure of Fe-N x active sites and significantly promoted mass transport during ORR. The resultant HP-Fe-N/C demonstrates superior ORR electrocatalytic activity, achieving a high half-wave potential of 0.75 V in 0.1 M HClO 4 and 0.89 V in 0.1M KOH aqueous solution. When applied as a catalyst for the cathode of PEMFCs, the HP-Fe-N/C delivers a remarkable peak power density of 528.4 mW cm -2 and a high retention rate of 88.5% of its initial current density after working for 10 hours. This work provides a new approach for the fabrication of well-controlled hierarchical porous carbon-based electrocatalysts for the PEMFC.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Youpu Zhao,Qing Sun,Jian Zhang,Jiawei Sheng
In this study, natural porous diatomite was utilized as a conciliatory carrier for the fabrication of Fe/N/C nano-clusters with assistance of binary molten salt of NaCl-ZnCl 2 under different annealing temperature and used to removal of norfloxacin (NFA). The sample Fe/D m900 (prepared at 900 °C) exhibited a high surface area and great catalytic performance for antibiotics in the presence of PMS. Over 97% NFA can be decomposed within 5 min and the final degradation rate reached 98%. Meaningfully, high-efficiency Fe/D m900 -PMS system was nearly impervious to pH values and inorganic cations in aqueous solution and could be a likely candidate for degradation of multiple contaminants in pharmaceutical outlet water. Furthermore, the other impacting variables such as catalyst dosage, PMS dosage, NFA concentration and initial pH were moreover explored towards debasement, and conceivable degradation pathways of NFA were presented through LC-MS. This work builds up a compelling procedure to synthesize super-dispersed Fe clusters, which may be amplified to other transition metal-based catalyst via molten salt.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
·
IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Lihui Xiao,Lei Du,Xiangyu Lu,Ruopeng Li,Jinqiu Zhang,Maozhong An
Extensive efforts have been devoted to active site designing for non-precious metal electrocatalysts; however, the porous structure engineering has been less emphasized, particularly for catalysts for gas diffusion electrodes, e.g., the cathode (oxygen reduction reaction, ORR) of Zn–air batteries. The desired porous structure is not only important for exposing high-density active sites but also beneficial for boosting mass transfer. Here, a dual-template strategy is proposed for constructing hierarchically porous structural Fe–N–C catalysts with dense active Fe–Nx moieties for the cathode of Zn–air batteries. The dual ZnCl2 and MgO hard templates jointly promote the formation of hierarchically interconnected carbon networks. The experimental results indicated both significantly improved active site accessibility and mass transfer, reasonably leading to enhanced ORR activity in conventional three-electrode cells. Particularly, it is deduced that the microporous structure is beneficial for dense active Fe–Nx moieties, while the ultra-macroporous structure is conducive to mass transfer during the ORR process. We further applied this dual-template-mediated catalyst in a real-world liquid Zn–air battery, which presents a high open-circuit voltage of 1.48 V and a remarkable energy density of 952.8 W h kgZn−1. Such robust battery performance is among the best compared with reported Zn–air batteries using non-precious metal catalysts. Particularly, a peak power density of 116.8 mW cm−2 is achieved in an all-solid-state Zn–air battery.
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高影响因子
ANALYST
·
2021
·Vol. 146
·期 14
·4557-4565
·
IF 4.616
Xiangyu Ma,Kun Qian,Onome Ejeromedoghene,Martha Kandawa-Schulz,Wei Song,Yihong Wang
Taking a composite of a nanomaterial and a signal molecule as a substrate material can provide a label-free electrochemical platform. Besides, the nanomaterial with a high catalytic activity towards the signal molecule can improve the sensitivity of the platform. Herein, a thionine functionalized Fe–N–C nanocomposite was employed as the substrate. Firstly, the electrocatalytic activity of Fe–N–C towards the electroreduction of thionine was explored. Then, an immobilization-free and label-free electrochemical platform for the determination of microRNA-21 based on Fe–N–C–thionine/Fe3O4@AuNPs was constructed. A magnetic glassy carbon electrode (MGCE) was used to keep the magnetic Fe–N–C–thionine/Fe3O4@AuNPs modified onto the surface of the MGCE. Fe–N–C and Fe3O4 nanoparticles can co-catalyze the electroreduction of thionine and a strong electrochemical reduction signal of thionine could be realized in the differential pulse voltammetry (DPV) test. Also, a catalytic hairpin assembly (CHA) reaction was utilized to enhance the sensitivity of the developed electrochemical biosensor. Besides, the developed biosensor shows excellent specificity and reproducibility in the test of human serum samples, indicating its wide application prospects in the early-stage diagnosis of tumors.
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DOI
PubMed
高影响因子
CARBON
·
2020
·
IF 8.821
Shuqi Hu,Wenpeng Ni,Daihui Yang,Chao Ma,Jiaheng Zhang,Junfei Duan,Yang Gao,Shiguo Zhang
Atomically dispersed Fe–N–C catalysts with additional Fe-containing nanoparticles including metal, carbides or oxides have shown great potentials towards oxygen reduction reaction (ORR) catalysis. However, the formation of these synergistically active nanoparticles and the effect of the porous carbon structures remain unclear. In this work, a novel single-atom-involved electrochemical catalyst, i.e. , Fe 3 O 4 nanoparticles encapsulated in atomically dispersed Fe–N–C (Fe 3 O 4 @FeNC) was reported. The optimized Fe 3 O 4 @FeNC exhibits excellent ORR activity with a half-wave potential of 0.890 V and a Tafel slope of 58.8 mV dec −1 , comparable with recently reported ORR catalysts and superior to these of commercial Pt/C. More importantly, the porous architectures not only affect the mass transfer and active sites, but casts huge influence on the nucleation of Fe 3 O 4 nanoparticles, the graphitization degree of the carbon support, the chemical environments of the elements, and the ORR catalytic pathways. Density functional theory calculations show stronger O 2 adsorption on Fe–N–C when supported on Fe 3 O 4 moieties, which may increase the reactant concentration for ORR and promote the overall activity. These findings will provide important references for the future understanding and design of single-atom-involved catalysts with enhanced electrochemical properties .
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xilong Wang,Qinghua Zhang,Hechun Jiang,Yadong Li,Hongwei Zhu,Lirong Zheng,Lin Gu,Han-Pu Liang
Pt-based intermetallic alloys with high activity and stability are promising for accelerating the cathodic oxygen reduction reaction (ORR) and large-scale application of proton exchange membrane fuel cells. So far, facile synthesis of Pt-based alloys in less time is desirable but still challenging. Herein, based on the traditional wet impregnation method, facile in situ reduction of H2PtCl6 and alloying with a hybrid nanostructure mainly doped with Fe single atoms as well as small amounts of Fe-based nanoparticles and oxides were developed to fabricate highly dispersed PtFe nanoparticles loaded on a mesoporous Fe–N–C support. Alloying of Pt derived from H2PtCl6 with various iron-based species existing in forms of single-atom, metallic, and oxide states was confirmed by systematic characterization, and the Fe content in the support is important for PtFe alloy formation, and the corresponding electrochemical performance promotion has been identified. The as-synthesized best-performance PtFe/Meso-PDA-5 catalyst delivered a high potential of 0.925 V at a current density of 3 mA cm–2 and achieved a high mass activity of 497.5 mA mgPt–1 at 0.9 V for the ORR in 0.1 M HClO4. More importantly, only 17.9% mass activity loss was observed after 10k potential cycles of the accelerated deterioration test. The present work provides a strategy for facile synthesis of Pt-based alloy nanomaterials for ORR catalysis and highlights the importance of supports in alloy formation.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Qian Liu,Chenye Zhang,Meimei Ren,Jinyi Wang,Leixin Feng,Yixuan Wang,Chuang Liu,Ningru Xiao,Haiming Zhang
Development of low Pt-loading electrocatalyst with enhanced activity towards oxygen reduction reaction (ORR) is highly demanded for widespread penetration of clean energy technologies. Heterointerface regulation can effectively optimize the electronic structure and intrinsic activity of the carbon supported Pt-based electrocatalyst to reduce Pt consumption. Here, by judicious choice of a sulfur-doped Fe-N-C (Fe-NS-C) as support, we construct a novel Pt/Fe-N-C heterointerface with sulfur incorporation and develop a hybrid electrocatalyst (denoted as Pt@Fe-NS-C) with ultralow Pt-loading (1.51 wt%). The incorporation of sulfur triggers the charge redistribution at the heterointerface and reduces the electron transfer from Pt to Fe-NS-C, prompting the electron density around Pt sites and boosting the electrocatalytic performance towards ORR (half-wave potential: 0.903 V; mass activity of 1.28 A mg −1 Pt at 0.9 V). In comparison, Pt species dispersed onto Fe-N-C without sulfur doping (Pt@Fe-N-C) are electron-deficient, which is not conductive to activate O 2 and results in inferior ORR activity. Zinc-air battery fabricated with Pt@Fe-NS-C as the cathode catalysts shows a large peak power density and a specific capacity of 806.7 mAh g −1 Zn . This work offers an effective way to tailor the heterointerface of hybrid or supported electrocatalyst with optimized electronic structures towards advanced electrocatalysis .
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高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 17
·6630-6638
·
IF 8.262
Fei He,Xinghua Chen,Yanfei Shen,Ying Li,Anran Liu,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
The development of efficient and low-cost non-precious-metal electrocatalysts such as Fe–N/C for the oxygen reduction reaction (ORR) is crucial for fuel cells and metal–air batteries. Here, we report a class of highly efficient Fe–N/C electrocatalysts derived from versatile imidazolium-based ionic liquids (ILs) with a halogen-coordinated iron anion. Without any supports, templates, or multi-step pyrolysis, the as-prepared Fe–N/C catalysts exhibited superior activity in the ORR to the state-of-the-art Pt/C in alkaline electrolytes by 44 mV in half-wave potential. More interestingly, owing to the versatile configuration of the imidazolium-based IL precursors, a diverse range of catalyst structures was successfully modulated. Based on this, it was clearly revealed that the electrical conductivity, type/amount of N dopants, and “effective porosity” (not the conventional total surface area) jointly determined the electrocatalytic activity. A pivotal radar chart is further proposed to successfully predict activity in the ORR merely from the structures of Fe–N/C catalysts. The proposed ILs platform would provide a valuable toolbox for the molecular design of precursors to tune the structures of Fe–N/C electrocatalysts towards excellent activity in the ORR in a highly flexible manner, and facilitate the long-term challenging study of relationships between processing, structure and activity.
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高影响因子
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