MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Tao Jiang,Weiling Luan,Yufeng Ren,Chenyao Fan,Qi Feng,Lyudmila Turyanska
Exploring an economical and efficient oxygen reduction reaction (ORR) is an essential but challenging field of study. Metal–organic frameworks (MOFs) have emerged as promising candidates for the preparation of porous catalysts. Here we propose a synergistic heat treatment (SHT) method to synthesize Fe–N–C-SHT catalyst with hierarchical porous hollow structures via a simple carbonization method by the synergistic heating of ZIF-8-Fe (ZIF-8 doped with Fe) and ZIF-67 in a tube furnace. Fe–N–C-SHT catalyst displays efficient ORR activity (half-wave potential ( E half ) = 0.88 V versus reversible hydrogen electrode (RHE) with a loading of 0.204 mg Fe-N-C-SHT cm −2 ), which is superior to that of Fe–N–C synthesized using individual heat treatment (IHT) ( E half = 0.84 V) and Pt/C catalyst ( E half = 0.86 V). We achieve enhanced catalytic properties, enhanced methanol tolerance, and long-term durability of the Fe–N–C-SHT catalyst in alkaline electrolyte . The improved ORR activity is attributed to the synergistic effect of Fe doping and optimized SHT methodology, which led to the formation of a highly porous catalyst with numerous active sites. The developed SHT method presents a novel route to fabricate Fe–N–C catalysts with hollow-mesoporous-microporous structures and high performance in ORR.
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高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Yabiao Pei,Weikang Zhu,Runfei Yue,Jie Yao,Xin Liu,Lianqin Wang,Junfeng Zhang,Yan Yin,Michael D. Guiver
Adjusting catalyst/ionomer agglomerate is crucial to a high-performance catalyst layer (CL), particularly for non-precious metal catalysts . As a sacrificial component, the solvent plays a vital role during the CL formation process and resulting microstructure, determining the performance of the anion exchange membrane fuel cells (AEMFCs). Here, solvent mixtures of isopropanol (IPA) and tetrahydrofuran (THF) are studied for the controllable construction of the Co/Fe–N–C CL. The results indicate that the aggregate state of the ionomers and catalysts and the final CL microstructure strongly depend on the ratio of IPA and THF. The CL prepared with IPA: THF = 1:2 (v/v) shows a homogeneous distribution of Co/Fe–N–C catalysts, embedded in the ionomer matrix, due to the fast volatilization and low viscosity of the catalyst ink. The Co/Fe–N–C CL with high moisture adsorption behavior and retention ability results in a high performance AEMFC with peak power density of 545.3 mW cm −2 at 80 °C. The obtained results can guide the rational design of microstructure in non-precious metal CLs for high-performance AEMFCs.
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高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2024
·
IF 6.7
Liu Weihao,Liu Qingtao,Wan Xin,Shui Jianglan
Non-precious metal electrocatalysts (such as Fe–N–C materials) for the oxygen (O 2 ) reduction reaction demand a high catalyst loading in fuel cell devices to achieve workable performance. However, the extremely low solubility of O 2 in water creates severe mass transport resistance in the thick catalyst layer of Fe–N–C catalysts. Here, we introduce silicalite-1 nanocrystals with hydrophobic cavities as sustainable O 2 reservoirs to overcome the mass transport issue of Fe–N–C catalysts. The extra O 2 supply to the adjacent catalysts significantly alleviated the negative effects of the severe mass transport resistance. The hybrid catalyst (Fe–N–C@silicalite-1) achieved a higher limiting current density than Fe–N–C in the half-cell test. In the H 2 –O 2 and H 2 –air proton exchange membrane fuel cells, Fe–N–C@silicalite-1 exhibited a 16.3% and 20.2% increase in peak power density compared with Fe–N–C, respectively. The O 2 -concentrating additive provides an effective approach for improving the mass transport imposed by the low solubility of O 2 in water.
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高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 29
·11357-11364
·
IF 8.262
Teng Liu,Pingping Zhao,Xing Hua,Wei Luo,Shengli Chen,Gongzhen Cheng
A simple Zn/Fe bimetallic zeolitic–imidazolite framework (ZIF) carbonization method is developed to synthesize an Fe–N–C hybrid with hierarchical nitrogen-doped porous carbons crossed by carbon nanotubes. Both the specific ratios of Zn/Fe in the bimetallic metal–organic framework (MOF) precursors and the selected annealing temperature are essential for the formation of this unique hybrid structure with good conductivity and exposure of more active sites. The resulting FeNC-20-1000 hybrid electrocatalyst exhibits excellent oxygen reduction reaction (ORR) activity, with a half-wave potential of 0.770 V comparable to that of the commercial Pt/C catalysts in acidic media, and a half-wave potential of 0.880 V, ca. 50 mV more positive than that of Pt/C for ORR in alkaline solution. More importantly, the as-prepared Fe–N–C hybrid exhibits much more stability for the ORR in both acidic and alkaline solutions than Pt/C, which makes it among the best non-noble-metal catalysts ever reported for ORR under acidic and alkaline conditions.
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Journal of Physical Chemistry C
·
2024
·
IF 3.3
Mingjun Xu,Zhao Jin,Meiling Xiao,Changpeng Liu,Wei Xing
Pyrolyzed iron and nitrogen codoped carbon materials (Fe–N–C) with atomically dispersed Fe-Nx sites have received extensive attention as a highly promising alternative to Pt for oxygen reduction reaction (ORR), yet there remains a considerable performance gap between them. To further improve the catalytic performance of Fe–N–C catalysts, we herein developed a microwave-assisted method to improve both the active site density (SD) and intrinsic activity, thus achieving outstanding ORR activity. The in situ generated Fe precipitation is beneficial to improve the doping efficiency of Fe and the subsequent formation of synergetic active sites, leading to increased SD. Both the X-ray absorption spectroscopy and operando Raman confirmed the copresence of atomic Fe moieties and nanoclusters, in which the nanoclusters synergically promote the activity of the single atomic sites. The enriched synergetic active sites endow the as-prepared catalyst with excellent performance by showing a current density of 42 mA cm–2 at 0.9 V in a proton exchange membrane fuel cell, approaching the DOE 2025 target. This work not only affords a highly active ORR catalyst but also provides a simple and potentially scale-up approach to Fe–N–C catalysts.
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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.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 7
·077512
·
IF 4.386
Wenhuang Xiao,Xiaolin Zhao,Luyin Lin,Jian Luo,Haipeng Yang
Sarcosine has been discovered as a better potential biomarker for Prostate cancer (PCa). Though many high-performance amperometric sarcosine biosensors have been reported, it is still difficult to accurately detect sarcosine because of the extremely low concentration and the presence of many electroactive interferents in human serum or urine. Since most of the reported sarcosine biosensors use platinum group metals (PGM) as catalysts, it is meaningful to explore other catalysts with higher catalytic activity. Metal-nitrogen-doped carbon (M–N–C) materials are considered as alternatives to precious metals. In this study, iron doped zeolitic-imidazolate-framework-8 (ZIF-8) composites were synthesized and calcined to obtain an Iron-nitrogen-doped Carbon (Fe–N–C) material, which has excellent catalytic activity. The sensitivity of the Fe–N–C modified sarcosine biosensor is 16.5 μA mM−1, (234.2 μA mM−1 cm−2), which is the highest one in recent reported works. It has a low limit of detection (LOD, 0.7 μM, S/N = 3), and an appropriate linear detection range of 2–37 μM. This work provides a new approach to prepare high performance sarcosine biosensors by improving the catalytic activity of the modifier of the sensor. It has great potential to be used as portable devices for the rapid detection of PCa.
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高影响因子
Environmental Science-Advances
·
2023
·Vol. 2
·期 5
·731-739
·
IF 0
Wen Wen,Yina Liu,Zhongping Li,Guangming Wen,Hung-Wing Li,Li Li
In this study, we report a simple pyrolytic strategy for N–C co-doped Fe-based nanoparticles (Fe–N–C) and exhibit their oxidase-mimicking and peroxidase-mimicking activity in a chromogenic reaction with 3,3′,5,5′-tetramethylbenzidine dihydrochloride (TMB) as a substrate. Structural analysis revealed that Fe–NX and Fe3C structures were formed with Fe-Imace coordination compounds as precursors and melamine as the nitrogen source, which provided abundant active sites for the Fe–N–C nanozyme. Interestingly, owing to the blocking effect triggered by π–π stacking between the tetracycline antibiotics (TCs) tetraphenyl skeleton and Fe–N–C, the substrate affinity of the Fe–N–C was significantly blocked, resulting in the solution fading. Under the optimum conditions, the UV absorption intensity versus the concentration of TCs was found to be linear over the range of 0.08–90 μM for tetracycline (TC), 0.1–80 μM for chlortetracycline (CTC) and 0.09–100 μM for oxytetracycline (OTC). The detection limits were 62 nM for TC, 85 nM for CTC and 88 nM for OTC. The Fe–N–C displayed good storage and long-term stability when stored at 4 °C for 30 days. In addition, based on its superparamagnetism, Fe–N–C can be effectively recycled and reused through an external magnetic field, avoiding secondary pollution.
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Frontiers of Environmental Science & Engineering
·
2025
·Vol. 19
·期 12
·1-17
·
IF 6.4
Wei Biao,Liu Daoqing,Peng Ran,Zhou Yi,Li Qianwei,Zhao Huazhang
The remediation of nitroaromatic-contaminated water systems remains a critical environmental challenge, creating the urgent need for cost-effective, non-precious metal catalysts to increase wastewater biodegradability. In this study, we present an Fe/N-functionalized three-dimensional porous carbon (Fe–N–C) catalyst synthesized via a straightforward pyrolysis approach that enables efficient nitrobenzene (NB) degradation via electrochemical and chemical reduction pathways. The high-temperature pyrolysis process facilitates the iron-catalyzed reconstruction of the carbon matrix, resulting in a hierarchically porous structure with increased graphitization and uniformly distributed macrocyclic Fe–N 4 coordination sites. These structural features give the Fe–N–C catalyst exceptional electron transfer kinetics, catalytic activity, and pH adaptability, surpassing conventional graphite (GR) and nitrogen-doped carbons (NPCs) in NB reduction. Systematic evaluation of the electrochemical reduction performance revealed that the Fe–N–C electrode achieved the highest NB removal efficiency. To further assess the versatility of the catalyst, a functionalized Fe–N–C/zero-valent iron (ZVI) composite was engineered by integrating Fe–N–C as a catalytic layer onto the reductant ZVI. Compared with ZVI alone, this composite markedly increased the NB reduction efficiency. These findings provide valuable insights into the electrochemical reduction process of Fe–N–C and new directions for the rational design of efficient nitrobenzene reduction systems.
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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.
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PubMed
高影响因子
DIAMOND AND RELATED MATERIALS
·
2026
·
IF 5.2
Yongzhi Zhao,Gengchen Bai,Wenhe Yu,Jianfang Liu,Baorui Jia,Xuanhui Qu,Mingli Qin
The development of efficient non-precious metal catalysts for the oxygen reduction reaction (ORR) is crucial for advancing sustainable energy technologies. Although single-atom Fe–N–C materials hold great promise, they are often limited by metal aggregation issues associated with conventional carbon supports. In this study, we propose a novel catalyst design that stabilizes Fe–N–C single-atom sites on a robust diamond-based matrix to fabricate a highly efficient electrocatalyst. With mild graphitization of the diamond surface to enhance its electrical conductivity during electrocatalytic processes, the Fe species are atomically dispersed and form coordinate covalent bonds with pyridinic N. In alkaline electrolyte, the Fe–N–D catalyst exhibits enhanced ORR activity, outperforming both pristine diamond and carbon black reference samples. Density functional theory (DFT) calculations reveal that the active Fe–N 4 –C configuration promotes kinetically efficient ORR by optimizing charge transfer and weakening the O O bond. This work integrates conductive sp 2 ‑carbon with a stable sp 3 -diamond core to establish a novel support for anchoring single-atom catalysts, providing a new substrate materials-design paradigm for electrocatalysis. Download: Download high-res image (124KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Wenhao Zhang,Chuanyi Zhou,Jiahao Cui,Canglou Liu,Yongfang Rao,Wei Yan
Current adsorbents for bisphenol A (BPA) require complex preparation and relatively low adsorption capacities. Here, a high-performance adsorbent (Fe-N-C) was synthesized from iron-modified zeolite imidazole frameworks-8 (ZIF-8) via pyrolysis. With an exceptionally high specific surface area of 1565.15 m 2 ·g −1 , Fe-N-C removed 90% of BPA within 10 min and achieved adsorption equilibrium within 3 h. Furthermore, Fe-N-C exhibited a maximum BPA theoretical adsorption capacity of 877.45 mg·g −1 (288 K). The adsorption kinetics and isotherms conform to pseudo-second-order kinetics and the Langmuir model. Fe-N-C also demonstrated excellent performance across a wide pH range (4–10) and in complex water matrix. The high adsorption capacity was primarily attributed to π-π interactions, along with hydrogen bonding, electrostatic interactions, and hydrophobic interactions. Notably, in addition to efficiently adsorbing BPA, Fe-N-C exhibited a high selectivity toward organic compounds with two benzene rings by π-π interactions, such as bisphenol B (BPB), 2,2-bis (4-aminophenyl) propane (BAPP) and diclofenac (DCF) due to the mediation of graphitized microdomains. This study provides a simple route to prepare high-capacity N-doped carbon adsorbents for the selective and rapid adsorption of specific structural pollutants.
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