JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Qiulin Li,Heng Liu,Long-Cheng Zhang,Hao Chen,Hongjiu Zhu,Yuanke Wu,Maowen Xu,Shu-Juan Bao
Fe-N and pyridinic-N generally are considered the active sites of Fe-N-C catalyst. In this featured work, small uniform Fe/N-rich polymer spheres are selected to prepare the Fe-N-C catalyst and study how the sintering atmosphere (NH 3 , Ar, and H 2 ) to engineer their products. The findings reveal that the sintering atmosphere greatly affected not only the composition , aggregate state, and morphology of Fe, but also the graphitization degree and pore structure of carbon. In addition, XPS results suggest that Fe-N-C-NH 3 possesses the highest Fe-N and pyridinic-N content. Combining its abundant pores, high graphitization, and large specific surface area, the catalyst obtained in NH 3 atmosphere delivers best ORR catalytic performance (E 0 = 0.97 V, E 1/2 = 0.85 V vs RHE), which is even comparable to commercial Pt/C (E 0 = 0.97 V, E 1/2 = 0.83V vs RHE). Moreover, the catalyst exhibits greater stability and methanol resistance than those of Pt/C.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2022
·
IF 16.383
Fei Xiao,Yian Wang,Gui-Liang Xu,Fei Yang,Shangqian Zhu,Cheng-Jun Sun,Yingdan Cui,Zhiwen Xu,Qinglan Zhao,Juhee Jang,Xiaoyi Qiu,Ershuai Liu,Walter S. Drisdell,Zidong Wei,Meng Gu,Khalil Amine,Minhua Shao
The poor durability of Pt-based nanoparticles dispersed on carbon black is the challenge for the application of long-life polymer electrolyte fuel cells. Recent work suggests that Fe- and N-codoped carbon (Fe–N–C) might be a better support than conventional high-surface-area carbon. In this work, we find that the electrochemical surface area retention of Pt/Fe–N–C is much better than that of commercial Pt/C during potential cycling in both acidic and basic media. In situ inductively coupled plasma mass spectrometry studies indicate that the Pt dissolution rate of Pt/Fe–N–C is 3 times smaller than that of Pt/C during cycling. Density functional theory calculations further illustrate that the Fe–N–C substrate can provide strong and stable support to the Pt nanoparticles and alleviate the oxide formation by adjusting the electronic structure. The strong metal–substrate interaction, together with a lower metal dissolution rate and highly stable support, may be the reason for the significantly enhanced stability of Pt/Fe–N–C. This finding highlights the importance of carbon support selection to achieve a more durable Pt-based electrocatalyst for fuel cells.
研究领域:
材料科学
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电化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
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
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电化学
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催化
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 13
·6058-6065
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IF 3.3
Xu Zhang,Jingxian Zhang,Shi Zeng,Haifan Wang,Yiling Bai,Huaming Hou,Ke Zhang,Bin Li,Guangjin Zhang
Iron–nitrogen-doped carbon (Fe–N–C) catalysts have been theoretically and experimentally demonstrated as one of the most promising materials to promote the oxygen reduction reaction (ORR), but they still have drawbacks in terms of stability and longevity. Herein, a novel strategy of loading Fe–N–C on cerium oxide cyanamide (Ce2O2CN2) is proposed to increase the density of active sites and improve the activity effectively. Ce2O2CN2 provides a Ce4+/Ce3+ redox pair to regulate the oxygen density on the catalyst surface, and the π–π interactions between Ce2O2CN2 and Fe–N–C are beneficial for interfacial charge transport. Consequently, Fe–N–C@Ce2O2CN2 shows excellent ORR activity with a half-wave potential (E1/2) of 0.89 V vs RHE and satisfactory long-term durability in an alkaline medium, and significantly outperforms commercial Pt/C. The Zn–air batteries made using the prepared catalyst exhibited a high peak power density of 119.35 mW cm−2. This study provides a new perspective for the application of platinum group-metal (PGM)-free catalysts in next-generation energy storage devices.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
研究领域:
生物化学
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医学诊断
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纳米技术
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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
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DOI
高影响因子
Fuel Cells
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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
JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Jiahao Yu,Jieyi Yu,Tongpan Ying,Xianguo Liu,Xuefeng Zhang,Dandan Han
Three main strategies for designing efficient microwave absorber includes the intrinsic dielectric/magnetic properties, the novel structure and the single atom doping. The Fe-N/C nanocomposites integrate the advantages of above three strategies into one system. In this work, the method for preparing Fe-N/C nanocomposite by calcining the FePc@ZIF-8 precursor under a flowing N 2 gas is described. Fe-N/C nanocomposites, displaying respectable dodecahedron-like morphology, have the merits of strong absorption ability, wide effective absorption bandwidth, thin thickness, and excellent microwave absorption efficiency, which are attributed to the synergistic effect of good electromagnetic loss capacity and proper impedance matching originating from intrinsic dielectric/magnetic properties, the novel structure and the single atoms (Fe and N) doping. Fe-N/C-24 composite delivers an optimal reflection loss of −30.98 dB, an effective absorption bandwidth of 5.04 GHz, the microwave absorption capacity of 87.61 dB GHz the absorption efficiency of 51.53 dB GHz/mm at 1.7 mm.
研究领域:
材料科学
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电磁学
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产品关联
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
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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
·
催化
·
材料化学
·
机械化学
·
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
·
生物启发设计
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYST
·
2020
·Vol. 146
·期 1
·207-212
·
IF 3.978
Wenjie Jing,Xiangkun Cui,Fanbo Kong,Wei Wei,Yunchao Li,Louzhen Fan,Xiaohong Li
Identifying the species and concentrations of antioxidants is really important because antioxidants play important roles in various biological processes and numerous diseases. Compared with an individual sensor detecting a single antioxidant with limited specificity, a sensor array could simultaneously identify various antioxidants, in which 3–5 types of nanomaterials with peroxidase-like activity are absolutely necessary. Herein, as a single-atom nanozyme, Fe–N/C with oxidase-mimicking activity was applied to construct a triple-channel colorimetric sensor array: (1) Fe–N/C catalytically oxidized three substrates 3,3′,5,5′-tetramethylbenzidine (TMB), 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS) and o-phenylenediamine (OPD) to produce blue oxidized TMB (oxTMB), green oxidized ABTS (oxABTS) and yellow oxidized OPD (oxOPD), respectively; (2) with oxTMB, oxABTS and oxOPD as three sensing channels, a colorimetric sensor array was constructed for simultaneously discriminating glutathione (GSH), L-cysteine (L-Cys), ascorbic acid (AA), uric acid (UA), and melatonin (MT), even quantifying concentrations (with GSH as a model analyst). The performance of the sensor array was validated through accurately identifying 15 blind samples containing GSH, L-Cys, AA, UA and MT in buffer solution and human serum samples, and also in binary and ternary mixtures. This work proved that fabricating a single nanozyme-based sensor array was a simplified and reliable strategy for simultaneously probing multiple antioxidants.
研究领域:
生物化学
·
医学诊断
·
纳米材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）