CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Tingting Xiang,Qingchao Zhu,Tanyu Zhou,Chenglong Chen,Ruibo Wang,Tieyu Hu,Bing Li,Ziwei Xu,Juan Yang
Graphical Fe−N−C catalysts, doped with phosphorus, show improved ORR activity. Fe-NPC catalyst exhibits high metal loading, excellent ORR performance (onset potential of 1.00 V, half-wave potential of 0.864 V), and promising application in Zn-air batteries (758.8 mAh g −1 Zn ). DFT calculations reveal that phosphorus enhances O 2 activation and reduces the energy barrier for the rate-determining step. Atomically dispersed iron and nitrogen co-doped carbon materials (Fe−N−C) represent promising non-precious metal catalysts for the oxygen reduction reaction (ORR), offering potential alternatives to noble metal-based benchmarks. In our study, we investigated the influence of phosphorus doping on the catalytic activity of Fe−N−C. The experimental research demonstrate that the doping of phosphorus significantly enhances the ORR activity. Specifically, the resulting Fe-NPC exhibits high metal loading and excellent ORR activity in 0.1 M KOH with an onset potential of 1.00 V and a half-wave potential of 0.864 V. Density functional theory (DFT) simulations reveal that phosphorus improves the electrocatalytic activity by activating O2 molecules and reducing the energy barrier (the hydrogenation reaction *OH→H2O) of the rate-determining step. Furthermore, Fe-NPC exhibits promising application prospects as an air cathode in Zn-air batteries, delivering a high maximum discharge power density of 180.3 mW cm −2 and outstanding discharge specific capacity (758.8 mAh g −1 Zn ) at a discharge current density of 10 mA cm −2 .
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Hao Wang,Xiaohao Liu,Guangyue Xu,Ziwei Guo,Ying Zhang
ABSTRACT Owing to Fe being the most abundant and least expensive transition metal on the earth, the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention. In this work, a series of N-doped C supported Fe catalysts (Fe-N-C) were prepared by co-pyrolysis of cellulose and ferric chloride under ammonia atmosphere. Characterization methods such as elemental analysis, atomic absorption spectroscopy, nitrogen adsorption-desorption isotherms, transmission electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were carried out to explore the physicochemical properties of the catalysts. Using hydrogenation of nitrobenzene as a model reaction, the catalysts prepared at different pyrolysis temperatures displayed different activities. Fe-N-C-700 exhibited the best activity among these catalysts, with the yield of aniline being up to 98.0% under 5 MPa H 2 at 120 °C after 12 h. Combined with the results of catalyst characterization and comparative tests, the transformation of Fe species and the generation of N-doped C, especially graphitized N-doped C, in the catalyst may be the main factors affecting the activity. A kinetic study was carried out and the apparent activation energy was obtained as 31.53 kJ/mol. The stability of the catalyst was also tested and no significant decrease in the activity was observed after 5 runs.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Fuel Cells
·
2022
·
IF 2.948
Yanqi Hao,Lin Ge,Siew Hwa Chan
Looking for non-noble metal catalysts with low cost, high activity, and high stability to replace platinum in oxygen reduction reaction (ORR) has aroused great concern. According to previous studies, Fe-N x /C material is one of the most promising non-noble metal catalysts for ORR. In this study, new Fe-N x /C material was synthesized by introducing CeO 2 and Fe 3 O 4 nanoparticles into a Fe-N x /C material derived from ZIF-8 as precursors. The new material was called CeO 2 -Fe 3 O 4 @Fe-N/C catalyst and the activity of the catalyst was found to be significantly improved in 0.1 mol L −1 KOH. The half-wave potential of CeO 2 -Fe 3 O 4 @Fe-N/C (0.892 V) is higher than that of Pt/C by 67 mV. In the stability test, the half-wave potential of CeO 2 -Fe 3 O 4 @Fe-N/C was only reduced by 4 mV after 5,000 cycles. The high performance is attributed to the introduction of CeO 2 and Fe 3 O 4 , which gives CeO 2 -Fe 3 O 4 @Fe-N/C enhanced electrocatalytic activity and long-term stability. This approach makes CeO 2 -Fe 3 O 4 @Fe-N/C a promising candidate for cathode catalysts in renewable energy conversion devices.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ruina Li,Xuwen Li,Qingcheng Liu,Hua Yue,Yang Meng,Yuanyuan Tian
With the continuous advancement of fuel cell technology, the exploration and development of highly efficient non - precious - metal catalysts for the oxygen reduction reaction (ORR) have emerged as a focal point of research. Fe–N–C catalysts have attracted much attention due to their excellent performance and low cost, and coupling single-atom catalysts (SACs) with atomic clusters (ACs) is an effective method to improve catalyst activity. This study used the pyrolysis method to synthesize iron atom catalysts (Fe–N–C SACs) and iron cluster coupled catalysts (Fe–N–C SACs/ACs) on ZIF-8 carbon support. It evaluated the catalyst performance through electrochemical testing. The experimental results showed that the introduction of Fe clusters improved the half-wave potential of the catalyst to 0.399 V, which represented an 8.2 % enhancement compared to the SAC catalyst and reached 87.1 % of that of the commercial Pt–C catalyst, and reduced the Tafel slope to 61.47 mV dec −1 , effectively improving the ORR activity of the catalyst. We constructed FeN 4 single atom catalyst models and FeN 4 /Fe 4 N 6 single atom cluster catalyst models using density functional theory (DFT), analyzed their electronic structures and reaction mechanisms, and revealed the mechanism of action of iron clusters. DFT calculations showed that iron clusters altered the charge distribution of FeN 4 sites, reducing the rate determining step (RDS) (OH desorption) energy to 0.5 eV, which promoted the desorption of products and the re-adsorption of reactants. As a result, the superior electrocatalytic performance of Fe–N–C SAC/AC is attributed to the synergistic effect between iron clusters and single atoms, which is influenced by the coordination environment and provides new ideas for designing efficient ORR catalysts.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yifan Zhang,Sylvestre Ndayiragije,Ming Chen,Xiaobo Wang,Lihua Zhu,Nan Wang
Fe- and nitrogen-doped carbonaceous (Fe-N-C) sites supported on MnO 2 (Fe-N-C@MnO 2 ) were prepared by a solvent-free mechanochemical method for peroxymonosulfate (PMS) activation to degrade norfloxacin (NFX). After a 50-min ball milling of iron(II) phthalocyanine (Fe( II )Pc) and MnO 2 at a weight ratio of 7.5 %, the obtained Fe-N-C@MnO 2 exhibited exceptional activity in PMS activation, achieving nearly complete degradation of NFX in 5 min with a rate constant of 0.62 min −1 . This rate constant was 11.5 and 28.2 times higher than that for milled MnO 2 (bm-MnO 2 ) and the mixture of Fe( II )Pc and MnO 2 , respectively. Alternative iron sources (FeSO 4 , FeCl 2 , Fe(III)-EDTA) and phthalocyanine showed no enhancement. Characterization revealed Fe-N-C@MnO 2 possessed abundant Mn 3+ , oxygen vacancies and Fe-N-C sites. Combined experimental and computational studies demonstrated Fe-N-C@MnO 2 simultaneously enhanced the 1 O 2 generation and facilitated the formation of SO 4 •− , •OH and O 2 •− , with contributions to NFX degradation following: 1 O 2 > •OH ≈ O 2 •− > SO 4 •− . This work establishes mechanochemical coordination engineering as a facile strategy for constructing high-performance metal-N-C hybrid catalysts.
研究领域:
环境科学
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催化
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材料化学
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机械化学
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水处理
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Yingfang Yao,Yong You,Gaixia Zhang,Jianguo Liu,Haoran Sun,Zhigang Zou,Shuhui Sun
Tuna is one of the most rapid and distant swimmers. Its unique gill structure with the porous lamellae promotes fast oxygen exchange that guarantees tuna’s high metabolic and athletic demands. Inspired by this specific structure, we designed and fabricated microporous graphene nanoplatelets (GNPs)-based Fe/N/C electrocatalysts for oxygen reduction reaction (ORR). Careful control of GNP structure leads to the increment of microporosity, which influences the O2 adsorption positively and desorption oppositely, resulting in enhanced O2 diffusion, while experiencing reduced ORR kinetics. Working in the cathode of proton-exchange membrane fuel cells, the GNP catalysts require a compromise between adsorption/desorption for effective O2 exchange, and as a result, appropriate microporosity is needed. In this work, the highest power density, 521 mW·cm–2, at zero back pressure is achieved.
研究领域:
材料科学
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生物启发设计
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yunpeng Zha,Xiaoxiao Sun,Zhengjun Xiong,Dandan Dong,Shili Li,Qinqin Wang,Minmin Liu
The porous carbon materials co-coordinated with Fe and N (Fe-N-C) were successfully synthesized through one-step pyrolysis with the zeolitic imidazolate framework (ZIF-8) as the precursor. Through systematic optimization of iron ion concentration during synthesis, the Fe-N-C-20 specimen exhibited optimal adsorption performance toward dibenzothiophene (DBT), demonstrating a maximum sulfur adsorption capacity of 22.14 mg S/g with a corresponding removal efficiency of 92 %. This superior performance can be primarily ascribed to the formation of Fe-S bonds anchored on Fe-N active sites, N-S interactions mediated by graphitic nitrogen species and appropriate pore size that allows access to thiophenic compounds. Furthermore, the experimental adsorption isotherms for DBT exhibited strong correlation with the Density Functional Theory (DFT) calculation. Additionally, the material's adsorption process followed pseudo-second-order kinetics and Langmuir isotherms of Fe-N-C, and the pseudo-second-order model shows the smallest RMSE (0.66), extremely low SSE (3.03) and AIC (-1.86), which further proves its excellent fitting ability. And the best balance between parameter efficiency and fitting performance. The high stability and recyclability of ZIF-derived Fe-N-C porous adsorbents contribute to sustainable industrial practices.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Liping Sun,Chao Li,Yong Yan,Yue Yu,Hao Zhao,Zijue Zhou,Feng Wang,Yi Feng
Single atom nanozymes (SAzymes) represent the state-of-the-art technology in nanomaterial-based catalysis, which have attracted attentions in catalysis, cancer treatment, disinfection and biosensing fields. However, numerous SAzymes suffered from low aqueous dispersion and without recognition capacity, which impeded their applications in bioanalysis . Herein, we engineered DNA onto SAzymes to obtain the DNA/SAzymes conjugates , which significantly improved the aqueous dispersion and recognition ability of SAzymes. We synthesized iron SAzymes (Fe–N–C SAzymes) as the catalytic nanomaterials, and investigated the interactions between Fe–N–C SAzymes and DNA. We compared A 15 , T 15 and C 15 adsorption of Fe–N–C SAzymes in HEPES containing 2 mM MgCl 2 . We found that 50 μg mL −1 Fe–N–C SAzymes produced nearly 100% A 15 adsorption, 90% T 15 adsorption and only 69% C 15 adsorption, indicating that adenine and thymine had higher adsorption affinity on Fe–N–C SAzymes. More importantly, DNA modification did not affect the peroxidase-like activity of Fe–N–C SAzymes and the bioactivity of the adsorbed DNA. Taking the advantage of the diblock DNA with one DNA sequence (adenine) binding to Fe–N–C SAzymes and the other DNA sequence (i.e., aptamer) binding to cancer cells, we designed Apt/Fe–N–C SAzymes for colorimetric detection of cancer cells, which offered new insights for the use of SAzymes in biomedicine .
研究领域:
生物医学
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纳米技术
·
催化科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 5
·053505
·
IF 4.386
Yanfang Song,Jinxiong Wu,Jiliang Zheng,Yiwei Sun,Andrei Ivanets,Guangming Du,Xintai Su
The doping of multiple heteroatoms can improve the electrochemical properties of carbon substrates. However, in existing studies, carbon, iron and nitrogen sources are generally mixed directly and then pyrolyzed for secondary activation. This tends to form aggregates of metal particles or metal oxides and requires the consumption of large amounts of alkali and energy. Therefore, there is an urgent need to develop an environmentally friendly technology capable of uniformly doping iron and nitrogen into carbon materials. In this work, porous Fe–N–C composites were prepared at 600 °C using potassium humate (HA-K) obtained from cotton straw by low-temperature pyrolysis as the carbon source, and urea-iron complexes formed by the pre-coordination of urea and Fe as the iron and nitrogen sources. In the absence of secondary activation, the best sample Fe-NHPC-2 had a good mesoporous structure with high specific surface area (889. 01 m2 g−1). It had a high specific capacitance of 256.8 F g−1 at a current density of 0.5 A g−1. The capacitance retention was 92.6% after 10,000 cycles at a current density of 10 A g−1. In the symmetric supercapacitor application, the energy density reached 33.16 Wh kg−1 when the power density was 600.2 W kg−1.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
ANALYST
·
2020
·Vol. 146
·期 3
·896-903
·
IF 3.978
Xiaolei Xie,Yufei Wang,Xiaobin Zhou,Junyang Chen,Mengke Wang,Xingguang Su
Single-atom nanozymes have drawn wide attention in bio-sensing for their remarkable merits such as low cost, high stability, and maximum atom utilization. Herein, a colorimetric strategy based on Fe–N–C single-atom nanozymes (Fe/NC-SAs) was established for the detection of alkaline phosphatase (ALP) activity. The Fe/NC-SAs prepared by pyrolysis have excellent peroxidase-like activity and can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue color product in the presence of hydrogen peroxide (H2O2). When ascorbic acid (AA) is added to the system, the blue color fades, and the absorbance has a linear relationship with the concentration of AA. Alkaline phosphatase (ALP) can catalyze the hydrolysis of ascorbic acid 2-phosphate (AAP) to produce AA. Thus, a strategy based on Fe/NC-SAs for the detection of ALP activity was established, which provided a linear range of 0.1–1.5 U L−1 and a limit of detection as low as 0.05 U L−1. Besides, Fe/NC-SAs showed high stability under harsh conditions. Moreover, an Fe/NC-SA-based assay was successfully validated using human serum samples for ALP determination with satisfactory results, and has broad prospects in the field of biosensing.
研究领域:
生物传感
·
医学检测
·
纳米材料
✓ 已验证
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 58
·14597-14603
·
IF 5.317
Xinghua Chen,Fei He,Yanfei Shen,Yiran Yang,Hao Mei,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
Graphical Interface effect : A study into the intrinsic role of carbon supports for Fe-N/C alternatives to Pt/C catalysts for oxygen reduction in fuel cells revealed that when immobilized on suitable support, the Fe−N/C demonstrated an improved mass J K that was comparable to that of Pt/C and higher than most reported M−N/C catalysts (see scheme). The mass kinetic current density (mass J K ) of most extensively reported M−N/C catalysts (M represents non-precious metal elements such as Fe, Co, and Cu), a potential alternative to noble metal catalysts in fuel cells, is poorer than that of commercial Pt/C. Thus, deep understanding of the intrinsic roles of carbon supports may contribute to the development of M−N/C catalysts from a practical point of view. Herein, the routinely used carbon supports, i.e. carbon black (CB) and carbon nanotubes (CNT) that have different morphology and crystallinity, were investigated to uncover the factors that affected the mass J K of Fe−N/C in electrocatalytic oxygen reduction. When immobilized on CB, the ionic liquids-derived Fe−N/C exhibited an enhanced mass J K (4.45 A g −1 at 0.80 V vs. RHE) by a factor of 2.14 times, comparable to that of Pt/C (5.79 A g −1 ) and higher than most reported M−N/C catalysts to our best knowledge. In contrast, the CNT support system showed no improvement. It was revealed that a compatible interface between the Fe−N/C precursors and the carbon supports was vital to ensure in-situ growth of a uniform catalyst layer on the supports during pyrolysis. This subsequently promotes the mass J K by exposing more embedded active sites and introducing favorable slit pores for effective mass-diffusion. This work would be promising to address the long-term overlooked challenge of the low mass J K of M−N/C catalysts in replacing noble-metal catalysts for practical fuel cell applications.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 41
·19506-19511
·
IF 6.97
Ying Li,Tong Liu,Wenxiu Yang,Zhijun Zhu,Yanling Zhai,Wenling Gu,Chengzhou Zhu
Non-Pt catalysts with excellent performance regarding the oxygen reduction reaction (ORR) have aroused enormous interest in recent years. Herein, we propose a dual-template method to synthesize a multiscale porous Fe–N–C (FeNC) catalyst. SiO2 and Zn are used as co-templates to produce a multiscale porous structure. Chitosan and glutaraldehyde are used as building blocks to fabricate the frameworks of the hydrogel. After lyophilization and annealing treatments, FeNC aerogel with a multiscale porous structure could be obtained. The as-prepared FeNC catalyst annealed at 900 °C (FeNC-900) exhibits a larger electrochemically active surface area and an improved ORR activity compared to FeNC annealed at other temperatures. FeNC-900 shows a superior ORR performance in comparison with that of commercial Pt/C in terms of the onset potential and half-wave potential, i.e., 0.959 and 0.837 V, which are 28 mV and 10 mV higher than those of Pt/C, respectively. Multiscale porosity is responsible for the outstanding ORR performance of FeNC-900. The electron transfer number of FeNC-900 for the ORR was calculated to be 3.95, which is comparable with that of Pt/C. In addition, the FeNC-900 catalyst possesses an excellent long-term duration and anti-poisoning capacity against methanol crossover. All these results endow the FeNC catalyst with tremendous potential for use in fuel cells.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）