MOLECULES
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2023
·Vol. 28
·期 7
·2879
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IF 4.6
Sensen Li,Yan Lv,Sawida Elam,Xiuli Zhang,Zhuojun Yang,Xueyan Wu,Jixi Guo
The rational design of morphology and structure for oxygen reduction reaction (ORR) catalysts still remains a critical challenge. Herein, we successfully construct defect-rich and hierarchically porous Fe-N-C nanosheets (Fe-N-CNSs), by taking advantage of metal-organic complexation and a mesoporous template. Benefiting from the advantages of high density of active sites, fast mass transfer channels, and sufficient reaction area, the optimal Fe-N-CNSs demonstrate satisfactory ORR activity with an excellent half-wave potential of up to 0.87 V, desirable durability, and robust methanol tolerance. Noteworthy, the Fe-N-CNSs based zinc–air battery shows significant performance with a peak power density of 128.20 mW cm−2and open circuit voltage of 1.53 V, which reveals that the Fe-N-CNSs catalysts present promising practical application prospects. Therefore, we believe that this research will provide guidance for the optimization of Fe-N-C materials.Keywords:electrocatalytic;Fe-N-C materials;oxygen reduction reaction;two-dimensional materials
研究领域:
材料科学
·
能源化学
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产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 23
·5557-5564
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IF 5.6
Yi Sheng,Hongmei Zheng,Jingting Hou,Wanying Zhang,Hong Chen,Luanjie Nie,Jing Zheng,Qingxue Lai
Fe–N–C materials as popular non-Pt group metal (non-PGM) electrocatalysts demonstrated huge potential for replacing Pt-based materials for efficient oxygen reduction reaction (ORR) electrocatalysis in acidic media. Herein, a metal–organic-framework (MOF)-based dual ligand strategy is proposed to develop advanced Fe–N–C materials with a controllable density of Fe-Nx sites and electrochemically active surface area, attributed to the synergistic effect from secondary ligand manipulation and Zn evaporation during pyrolysis. As a result, the optimized catalyst exhibits an ORR half-wave potential of 0.747 V vs. RHE and long-term stability with only a 29 mV negative shift after 3000 potential cycles in 0.5 M H2SO4 electrolyte. More far-reaching, this MOF-based dual ligand strategy opens a novel avenue to the precise fabrication of efficient catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yanjie Niu,Jie Xu,Liqing Chen,Sixi Guo,Fanhui Guo,Yixin Zhang,Jianjun Wu
As a typical coal-based solid waste, coal gasification fine slag (GFS) will have an annual discharge of more than 50 million tons in 2025 in China alone. However, the difficulty of its resource utilization lies in the precise separation of carbon and ash due to their complex distribution pattern. There is an urgent need to develop GFS-based materials for comprehensive utilization of carbon and ash. In this study, a combined process of acid leaching and pyrolysis was designed, in which active metal iron was leached from ash and immobilized on the surface of residual carbon in the form of Fe-N-C. The unique structure of Fe-N doped carbon/ash synergistically improved the efficiency of electrocatalytic degradation of organic wastewater by 72.78 ± 1.37%. The hierarchical porous structure of residual carbon considerably enhanced the accessibility of ash catalytic sites. Abundant ash defects and Fe-N active sites promoted the conversion of free radical precursors to reactive oxygen species (ROS). The removal rate of various organic wastewater within 35 min reached more than 100 ± 1.83% %, with excellent electrocatalytic performance and pH adaptability. Fe-NCPE had a high specific surface area (318.36 m 2 ·g −1 ), orderly graphite phase (002 crystal surface size 1.3 nm), and abundant catalytic sites. We also proposed the catalytic mechanism by combining molecular simulation with experiments. The high adsorption capacity above 24.07 ± 0.12 mg·g −1 ensured the continuous and rapid supply of pollutants and H 2 O 2 near the catalytic site·H 2 O 2 was converted into ROS mainly composed of hydroxyl groups through the valence state change of aluminum or Fenton-like reaction of nitrogen-linked iron. The ROS then attacked organic molecules to degrade pollutants. The above two processes corresponded to two cyclic catalytic reactions. Therefore, this study provides an innovative and promising approach for comprehensive utilization of carbon and ash in GFS.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Wei Wu,Wei Zhang,Yu Long,Jiaheng Qin,Jiantai Ma
Carbon material derived from certain MOF usually still has plenty of microporous structures, the mass transfer process is severely limited. In this work, in the assistance of dicyandiamide, nitrogen doped carbon confined atomically dispersed Fe species (Fe–N–C) with interconnected mesoporous pores by a facile one-step pyrolysis process of Fe-doped zeolitic imidazolate framework (Fe-doped ZIF) is prepared. Through simply adjusting the amount of dicyandiamide added, Fe–N–C with various morphologies, pore structures and chemical compositions could be obtained. The specific surface area of the materials increases first and then decreases with the increase content of dicyandiamide, and the pore structure also changes accordingly. Fe–N–C possesses the largest specific surface area with interconnected pore structure when the mass ratio of dicyandiamide to Fe-doped ZIF reaches 1:1 (Fe–N–C–1). And Fe–N–C–1 shows the optimal catalytic activity compared with other catalysts for the transfer hydrogenation of halonitrobenzenes. Moreover, the Fe–N–C–1 exhibits good stability and could be reused without obvious decrease of catalytic activity. This work may afford certain thought for rationally designing high-performance catalysts derived from MOF .
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 12
·3814-3823
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IF 7.683
Hanfeng Zhou,Zhibo Deng,Tianbao Liu,Tao Liu,Lijuan Zhang,Xintai Su,Zhang Lin
The science linking thermochemical conversion of large-scale industry oily sludge with applied materials has been improved in the last ten years. However, with the traditional converting methods it is hard to precisely control the composition and structure of oily sludge-based products during pyrolysis due to the complexity of the composition of the oily sludge. Here, a chlorinating calcination method using sodium chloride (NaCl) as a chlorinating salt and template was first developed to prepare porous Fe–N–C materials (FCN-500) through pyrolysis of oily sludge containing iron-bearing minerals and pyridine. The formation mechanism of FCN-500 was proposed, where iron ions (Fe3+) from the inorganic component (anorthite) in the sludge were rapidly dissociated with the assistance of NaCl, followed by coordination with the organic component (pyridine nitrogen) in the oily sludge to form the pyridine nitrogen–iron ((C5H6N)n–Fe) complex, and then carbonization. As-obtained FCN-500 exhibited higher specific capacitance (286.3 F g−1 at a current density of 0.5 A g−1), enhanced energy density (33.5 W h kg−1 at a power density of 606.1 W kg−1) and more excellent stability and durability (more than 80.1% capacitance retention after 10 000 cycles) compared with two other electrodes. The reasonably better performance of the obtained FCN-500 in supercapacitors (SCs) is attributed to its large surface area, hierarchically porous channels, high conductivity, and unique Fe–N–C structure. Therefore, this work not only provides a feasible way to solve the bottleneck problem in sludge pyrolysis, but also provides a method to design large scale porous Fe–N–C materials for practical applications.
研究领域:
环境科学
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材料科学
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能源科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 11
·1438
·
IF 4.501
Guolei Liu,Xue Li,Qing Wang,Kuizhao Sun,Chuping Lee,Yue Cao,Weimeng Si,Haoran Wei,Zhongfang Li,Fagang Wang
In the work, a pig-blood-derived mesoporous carbon (BC) was prepared as a novel Fe-N-C material for the electrochemical sensor to detect hydrogen peroxide. Because of the unique nanostructure of Fe-BCs with rough surface structure, hierarchical pores, and high graphitization degree, the Fe-BCs, as a kind of advanced electrode material, exhibited remarkable performance in electrocatalysis. The sensor based on Fe-BCs exhibited an extra-long range from c and a detection limit of 0.046 μM (S/N= 3). The synthesis of low-cost, advanced carbon-based electrode materials from environmentally friendly pig blood for electrochemical sensor construction is a promising approach.
研究领域:
生物医学工程
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材料科学
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分析化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Rui Li,Xiaoxuan Sun,Ling Yang,Panpan Zhao,Jianguo Zhao,Jiao Ding,Shuangli Wu,Chenguang Li,Hao Liu,Shaojun Dong
Curbing the rapid structural degradation of Fe-N-C materials during acidic oxygen reduction reaction (ORR) has been a long-standing challenge in commercializing ORR-based device with long-term stability. Herein, structural deactivation is effectively inhibited via optimizing interfacial Fe-O dipole by introducing the second Fe atom. The elaborately designed Fe double-atom catalysts (Fe DACs), featuring Fe₂N₆ motifs, induce a shift in O 2 adsorption geometry from end-on to bridge configurations for reorienting interfacial Fe-O local dipole ( μ L ) to relieve demetallation. Hence, Fe DACs achieve enhanced operational stability by 10.4 and 31.2 times over Fe 1 N 4 in both single electrode systems and H 2 O 2 -O 2 fuel cells. In-situ measurements and theoretical simulations reveal the origin for the suppression of structural degradation is due to that the optimized Fe-O μ L reduces the tensile stress exerted by the electric field on the Fe-N bond, coupled with intrinsically stable electronic structure in Fe₂N₆ during dynamic structural evolution to stabilize Fe-N bonds.
研究领域:
催化化学
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电化学
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材料科学
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能源化学
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 16
·9543-9549
·
IF 4.036
Tanlun Wang,Chenxiang Sun,Yong Yan,Fan Li
Metal–N–C-based catalysts prepared by pyrolysis are frequently used in the oxygen reduction reaction (ORR). Zeolitic imidazolate frameworks (ZIFs), a type of metal organic framework (MOF), are selected as precursors due to their special structure and proper pore sizes. A series of Fe–N–C catalysts with different concentrations of 2-methylimidazole were prepared with a simple solvothermal-pyrolysis method, and the transformation productivity, morphology and ORR activity were investigated. It was found that the Fe–N–C catalyst with a 2-methylimidazole concentration of 0.53 mol L−1 had the best performance. In 0.1 M KOH solution, the half-wave potential was 0.852 V (vs. RHE), with the highest electrochemically active surface area (ECSA) of 94.1 cm2, and the ORR reaction was dominated by a 4-electron process. The current only decreased by 10.5% after 50 000 s of chronoamperometry (CA), while the half-wave potential only decreased 20 mV in 3 M methanol. Additionally, this catalyst cannot be poisoned by Cl− and SO32− ions in the ORR process. Finally, some typical ions including SCN−, Fe(CN)63− and Fe(CN)64− were used to inhibit the active sites, and it was determined that Fe(II) is the real active species. The series of synthesis and testing experiments has significance in guiding optimization of the synthesis conditions and analysis of the mechanism of active sites in Fe–N–C materials.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Ke Qin,Zhenye Zhu,Fei-Xiang Ma,Jiaheng Zhang
Single atomic metal N C materials are the most promising candidates to replace platinum-group-metal (PGM) catalysts for the oxygen reduction reaction (ORR), and show a broad application prospect in long-life rechargeable Zn-air batteries. Iron-nitrogen co-doped carbon hollow nanospheres (Fe N C/HSs) were fabricated via the self-polymerization of dopamine coated on removable SiO 2 nanospheres and spontaneous chelation of Fe 3+ ions, followed by rational pyrolysis and template removal processes. Benefitted from unique micropores hollow structures and highly exposed Fe-N x active sites, the relevant Fe N C/HSs exhibited satisfied oxygen reduction performance (e.g. half-wave potential: 0.87 V), endowing the Fe N C/HSs assembled Zinc-air battery delivering a high power density of 157 mW cm −2 and large specific capacity of 805 mA h g −1 .
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hao Xu,Ruopeng Li,Huan Liu,Weiyan Sun,Jie Bai,Xiangyu Lu,Peixia Yang
Atomically dispersed iron–nitrogen-carbon (FesbndNsbndC) materials have been considered ideal catalysts for the oxygen reduction. Unfortunately, designing and adjusting the electronic structure of single-atom Fe sites to boost the kinetics and activity still faces grand challenges. In this work, the coordination environment engineering is developed to synthesize the Fe SA /NSC catalyst with the tailored N, S co-coordinated Fe atomic site (Fe-N 3 S site). The structural characterizations and theoretical calculations demonstrate that the incorporation of sulfur can optimize the charge distribution of Fe atoms to weaken the adsorption of OH* and facilitate the desorption of OH*, thus leading to enhanced kinetics process and intrinsic activity. As a result, the S-modified Fe SA /NSC exhibits outstanding catalytic activity with the half-wave potentials ( E 1/2 ) of 0.915 V and 0.797 V, as well as good stability, in alkaline and acidic electrolytes, respectively. Impressively, the excellent performance of Fe SA /NSC is further confirmed in Zn-air batteries (ZABs) and fuel cells, with high peak power densities (146 mW cm −2 and 0.259 W cm −2 ).
研究领域:
材料科学
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电化学
·
能源存储与转换
✓ 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）