SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhenyu Yan,Xiuyun Zhao,Chenkai Zhong,Wenyu Gao,Yujie Feng,Jia Liu
FeNx sites show significant superiority in the degradation of antibiotic contaminants, but there are difficulties in successfully constructing highly dispersed FeNx sites. In this work, Fe-N/C catalysts doped with hierarchical ordered pores structure and FeNx active sites were prepared by metal node exchange strategy. Among them, Fe-N/C-2 had more excite species for peroxymonosulfate (PMS) owing to the synergy between Fe and N coordination, which achieved 89.36 % tetracycline (TC) removal rate within 20 min, and its reaction kinetic ( k = 0.245 min −1 ) is 7.66 times more than original PMS system. Moreover, the material exhibited excellent activation performance in a variety of complex water environments, such as the coexistence of multiple anions, strong acids and alkalis (pH = 2.90 ∼ 10.73), and natural organic matter interference. Chemical bond detection confirmed the successful formation of FeNx sites, free radical trapping experiments showed that FeNx was the main catalytic site, and 1 O 2 was the main active component. Furthermore, the reaction principle of the FeNx site catalyzing the production of 1 O 2 from PMS was revealed in detail through mechanism exploration. Next, the probable pathways of TC decomposition were elaborated in terms of the intermediates identified by Liquid Chromatograph Mass Spectrometer (LC-MS). This study emphasized the significant potential of synthesizing Fe-N/C catalysts with activated FeNx sites, elucidated mechanism of FeNx in PMS activation, and confirmed its feasibility in TC degradation.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Haoyang Wu,Zhilong Tan,Bin Miao,Hailong Hu,Sanying Hou
In this work, Fe, N co-doped hierarchical porous graphite-like carbon with carbon-encapsulated Fe/Fe 3 C@ Fe-N-C was synthesized by a facile solid-phase synthesis strategy, and was employed as an efficient catalyst to activate peroxymonosulfate (PMS) for oxidation of tetracycline (TC). The optimal Fe-N/C 800 outlined a highly catalytic performance in activating peroxymonosulfate (PMS) with TC decomposition rate reaching 89.2 % in 20 min at ultra-low catalyst dosage. Meanwhile, the effect of operating parameters was also investigated in order to evaluate the potential of using Fe-N/C 800 in practical applications. In addition, the characterization analysis and experiments results elucidated that graphitic N, pyridinic N, C O, Fe 3 C, Fe 0 and FeN 4 were considered as the main reactive species promoting the PMS activation to generate reactive oxygen species (ROS) (including singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 •- ) and hydroxyl radical (•OH)). The electron paramagnetic resonance (EPR) experiments and radicals quenching analyses further demonstrated that the non-radical species singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species. Moreover, the TC degradation pathways were presented by LC-MS. Ultimately, the toxicity of the intermediate products were also investigated by ECOSAR system.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Zhiyan Huang,Pingxiao Wu,Chenhui Liu,Meiqing Chen,Shanshan Yang,Zhi Dang,Nengwu Zhu
Understanding the origin of high activity of graphene layers encapsulated Fe-N-C catalysts in Fenton-like reaction is critical, but still challenging for developing catalysts with high activity and durability. Therefore, we prepared a highly active Fe-N-C catalyst (Fe x Mn y -Fe@NCs) containing FeN 4 coordination to activate peroxymonosulfate (PMS) toward 4-aminobenzoic acid ethyl ester (ABEE) degradation, and revealed the multiple catalytic reaction sites by investigating the composition and the structure of the catalyst. The relationship between the catalytic degradation performance and multiple catalytic reaction sites was performed on the basis of both experiments and density functional theory (DFT) calculations. The catalytic performance of Fe 2 Mn 1 -Fe@NCs was found to show optimal catalytic degradation performance. Pyrrolic N served as adsorption site as well as singlet oxygen generation site to promote the catalytic degradation. Fe-pyridinic N-C acted as hydroxyl radical and sulfate radical generation site. Both singlet oxygen and superoxide radical were dominated the catalytic reaction. The insight achieved from this study may be further applied to other Fe-N-C catalysts design and further efficient organic pollution remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
研究领域:
化学
·
材料科学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
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
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 45
·20762-20769
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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.
研究领域:
材料科学
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电化学能源
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2021
·Vol. 146
·期 14
·4557-4565
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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.
研究领域:
生物传感技术
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分子诊断
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纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
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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.
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
Nanoscale
·
2024
·Vol. 16
·期 48
·22273-22282
·
IF 5.8
Feng Li,Kairen Zhao,Yan Jin,Baoxin Li
Currently, water treatment usually requires additional light illumination or oxidants for the degradation of organic pollutants, which increases the costs and is not conducive to practical application. In this study, carbon vacancy-modified Fe–N–C single-atom catalysts (Cv-Fe–N–C SACs) were prepared through one simple acid-etching and pyrolysis process. Interestingly, we found that Cv-Fe–N–C SACs could degrade organic pollutants without any external assistance (such as oxidants or light illumination). The Cv-Fe–N–C SACs could remove over 99% of Rhodamine B (RhB) within 10 min at room temperature. The degradation of organic pollutants with the Cv-Fe–N–C SACs was attributed to their ability to activate dissolved oxygen for producing superoxide (O2˙−). In addition, the catalysts showed high activity over a broad pH range (3–11) and held rather good stability after 5 recycles. This study proved that the Cv-Fe–N–C SACs are highly efficient catalysts for degrading organic pollutants. These catalysts have the potential to make sewage treatment more efficient and less expensive.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Wenlu Yang,Bingran Guo,Ziyu Guo,Xue Wang,Yanli Zeng,Jianing Guo,Mingxing Wu
Designing low-cost and high-efficiency non-noble metal electrocatalysts for the oxygen reduction reaction (ORR) is critical for the development of renewable and sustainable energy devices. It is of essential importance to precisely design and rationally adjust the porous morphology and nanostructure of catalysts to improve mass transfer and the accessibility of active sites. Herein, we elaborately designed a unique hollow hierarchical porous carbon nanofiber with Fe3O4/Fe–N–C sites anchored as a high-efficiency electrocatalyst for ORR. The hollow porous carbon nanofibers (HPCNFs) were prepared via a facile convenient coaxial electrospinning technology to fabricate the hollow carbon nanofibers and through zinc nitrate-assisted pyrolysis to form a hierarchical porous structure. Benefiting from its unique hollow porous construction, facilitated mass transfer, and highly accessible active sites, the optimized Fe-HPCNFs catalyst exhibited significant ORR performance and stability, with a half-wave potential of 0.89 V outperforming the commercial catalyst (20% Pt/C). Remarkably, Zn–air batteries assembled with Fe-HPCNFs achieved excellent activity with a robust peak power density of 172 mW·cm–2 and a high specific capacity of 905.4 mAh·gZn–1. Furthermore, the ORR mechanism was investigated by density functional theory calculations, demonstrating that the synergistic effect of Fe3O4 nanoparticles and Fe–N–C active sites can effectively boost the electrocatalytic activity for ORR.
研究领域:
材料科学
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电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Guangchao Li,Youbin Zheng,Hao Guo,Ze Li,Guohao Zhu,Liang Dong,Xin Liu,Jianbing Zang
In this paper, we present a method to enhance the stability of Fe–N–C electrocatalysts, known for their significant oxygen reduction reaction (ORR) activity and positioned as promising alternatives to commercial noble metal-based catalysts. Despite the favorable ORR activity, Fe–N–C suffers from inadequate stability in acidic media, primarily attributed the loss of active FeN 4 sites resulted from Fe-demetalation. However, recent investigation reveals that pyridine N exhibits remarkable stability in retaining Fe atoms. To address this, we achieved a high proportion of pyridine N doping in carbon nanofibers through a process involving nano-SiO 2 shell coating and electrospinning. The nano-SiO 2 shell coating method demonstrates efficacy and versatility in transforming pyrrole-type FeN 4 into pyridine-type FeN 4 , irrespective of the origin material being trivalent or divalent Fe, whether organic or inorganic.
研究领域:
电化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xinfa Cai,Fei Ma,Jun Jiang,Xianglong Yang,Zhaowei Zhang,Zelang Jian,Meijuan Liang,Peiwu Li,Li Yu
Sensitive, on-site and multiple detection of mycotoxins is a vital early-warning tool to minimize food losses and protect human health and the environment. Although paper-based lateral flow immunoassay (LFIA) has been extensively applied in mycotoxins monitoring, low-cost, portable, ultrasensitive and quantitative detection is still a formidable challenge. Herein, a series of Fe-N-C single-atom nanozymes (SAzymes) were synthesized and systematic characterized. The optimal Fe-N-C SAzyme with highly efficient catalytic performance was successfully used as both label and catalyst in lateral flow immunoassays for mycotoxin detection. By taking advantage of the catalytic amplified system, the qualitative and quantitative detection can be easily and flexibly done via observing the test lines by naked eyes or a smartphone, with the limit of detections (LODs) of 2.8 and 13.9 pg mL −1 for AFB 1 and FB 1 , which were respectively over 700- and 71,000-fold lower than the maximum limit set by the European Union. Besides, underlying catalytic mechanisms and the active sites of the Fe-N-C SAzyme are also investigated by DFT simulation. This work not only provides a promising detection strategy for the application of advanced SAzymes but also offers experimental and theoretical guidelines to understand the active centers of Fe-N-C SAzymes and the catalytic process.
研究领域:
食品安全
·
生物化学
·
环境健康
✓ 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）