FUEL PROCESSING TECHNOLOGY
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2022
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IF 8.129
Qin Wen,Dongxu Tian,Zequan Zeng,Fei Qi,Zhanggen Huang
Fe-N-C catalysts with magnetism were successfully synthesized through one-step heat treatment of ferrosoferric oxide and covalent organic frameworks composite (Fe 3 O 4 @COF) as heterogeneous catalysts for persulfate (PS) activation and 2,4-dichlorophenol (2,4-DCP) degradation. The morphologies, compositions and active sites were adjusted by changing the pyrolysis temperature. The catalyst prepared at 900 °C showed excellent activity with 2,4-DCP removal of 90% in 60 min, recycling convenience and regeneration stability. Large surface area (342 m 2 g −1 ) and hierarchical porous structure benefited PS activation. It was proved that the radical and non-radical mechanisms coexisted in Fe-N-C-900/PS system with the results of quenching and electrochemical experiments. Roles of graphitic N and Fe-N X were distinguished. Graphitic N and Fe-N X sites palyed an prominent part in the non-radical activation process , in which Fe-N X was closely related to the electron transfer activation mechanism. Density functional theory (DFT) calculation further verified that the Fe N 2 was the key site for PS activation. 2,4-DCP degradation was proved to be a toxicity-attenuation process according to the biotoxicity analysis. The effects of several operating parameters and degradation of different model pollutants were also systematically evaluated, and possible activation mechanism was proposed.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Mahmood ul Haq,Dong-Hui Wu,Zeeshan Ajmal,Qi-Dong Ruan,Shahid Khan,Lu Zhang,Ai-Jun Wang,Jiu-Ju Feng
In pursuit of advanced nanocatalysts with multifunctionality, cost-effectiveness and durability for water splitting and zinc-air batteries, we unveil a novel strategy by combination of electrochemically etched Nb 4 C 3 T x -MXene nanosheets with Fe-N-C single-atom catalyst. The resultant Fe-N-C/Nb 4 C 3 T x demonstrates exceptional electrocatalytic performances for the ORR ( E 1/2 = 0.911 V), OER ( η 10 = 1.52 V), and HER ( η 10 = 91 mV) in the alkaline media. Besides, the catalyst shows excellent application in water splitting electrolyzer, only requiring 1.58 V for a current density of 10 mA cm −2 . Further, the Fe-N-C/Nb 4 C 3 T x assembled battery displays an open-circuit voltage of 1.51 V, a higher peak power density (136 mW cm −2 ), a narrower polarization gap (0.85 V), and remarkable stability (660 cycles over 220 h), surpassing the Pt/C + RuO 2 based counterpart. Our study integrates DFT calculations to guide the catalyst design, laying the foundation for development of reliable and effective trifunctional catalysts in advanced energy-related systems.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Wen-Jun Niu,Ru-Ji Li,Wei-Wei Zhao,Ying-Yun Yan,Er-Peng Feng,Jiang-Lei Chen,Bing-Ni Gu,Ming-Jin Liu,Yu-Lun Chueh
Herein, a soft-template strategy involving the cationic surfactants has been successfully applied to size-controlled synthesis of hierarchical porous Fe-N/C for the first time. Specifically, a small amount of Fe and cationic surfactants can be uniformly doped into the zinc-based zeolite imidazole framework (ZIF-8) crystal particles and the cationic surfactants play a critical role in the formation of hierarchically porous Fe-ZIF-8@surfactant precursors. When the Fe-ZIF-8@surfactant is subsequently pyrolyzed, atomically dispersed Fe-N x coordination structures can be in-situ converted to Fe-N/C, while the cationic surfactants decompose to form a carbon matrix to encapsulate the active sites, thereby preventing the aggregation of nanoparticles to a certain extent. As a result, the combined Fe nanocrystals and atomically dispersed Fe-N x in the graphitic carbon matrix generate a synergistic effect to boost the electrocatalytic behaviors with a more positive half-wave potential (0.92 V) for oxygen reduction reaction (ORR) and a lower overpotential (420 mV at 10 mA cm −2 ) for oxygen evolution reaction (OER). As a proof of concept, the Fe-N/C@TTAB based zinc-air batteries (ZABs) present an outstanding peak power density (107.9 mW cm −2 ) and a superior specific capacity (706.3 mAh g −1 ) with robust cycling stability over 900 cycles for 150 h, which are better than the commercial Pt/C + IrO 2 based ZABs.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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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.
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高影响因子
Biomaterials Advances
·
2025
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IF 6
Yang Guo,Xinyu Gao,Fang He,Sihan Wang,Jingting Li,Fan Yang,Zihan Zhou,Changsong Dai,Zhaohui Wen
When nano-enzymes are used in tumor therapy research, they usually exhibit only a single enzyme activity, which limits their therapeutic effect in hypoxic tumors. This paper designs a hyaluronic acid (HA)-modified Au-Pt-Fe trimetallic flower-like nanomaterial for tumor cascade catalysis integrated with low-temperature photothermal therapy. GOx activity exhibited by AuPt nanoparticles converts glucose in tumor cells into gluconic acid and H 2 O 2 . This process not only deprives tumor cells of their energy source but also produces H 2 O 2 . Iron single-atom nanomaterials can exhibit excellent CAT and POD activities, catalyzing H 2 O 2 reactions in tumor cells. Among them, a portion of H 2 O 2 is converted to O 2 by the activity of nanozyme CAT, which is used to alleviate tumor tissue hypoxia and serve as a substrate for the GOx-like activity reaction of AuPt NPs. The H 2 O 2 is continuously produced by the glucose catalytic reaction, and a portion of it can further decompose into toxic OH through POD activity, contributing to tumor cell destruction. The glucose-H 2 O 2 -O 2 cycle reaction is realized, that is, the self-supply of H 2 O 2 and O 2 in the catalytic process within tumor cells. The introduction of AuPt nanoparticles enhances the photothermal conversion ability of the material. By using near-infrared light irradiation, mild-temperature photothermal therapy (m-PTT) can be achieved, which further improves the treatment effect while protecting surrounding tissues. This work expands the application of multi-metal nanomaterials in cascade catalysis combined with low-temperature photothermal therapy, providing a novel strategy for integrated tumor treatment.
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JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Danke Chen,Jiapeng Ji,Zhongqing Jiang,Min Ling,Zhongjie Jiang,Xinsheng Peng
Transition metal-nitrogen-carbon (M/N/C) catalysts, Fe/N/C in particular, with low cost, good tolerance to methanol and promising activity has great potential to replace Pt-based catalysts in oxygen reduction reaction (ORR). However, for metal atoms are easy to migrate and agglomerate during pyrolysis , it still remains a challenge to rationally design precursors to synthesize highly active M/N/C without significant agglomeration of metal sites. In this work, we propose a molecular-confinement strategy to synthesize sub-nano Fe/N/C catalysts by confinement [Fe(CN) 6 ] 3- in zeolitic imidazolate framework-8 (ZIF-8) crystals to minimize the agglomeration of Fe atoms during pyrolysis . The half-wave potential of the prepared sub-nano Fe/N/C is 40 mV superior to that of commercial 20% Pt/C in alkaline medium . Besides, it has electron transfer number close to 4.00, with below 0.5% H 2 O 2 yield, excellent long-term stability with only −5 mV shifts after 10000 cycles, and superb methanol tolerance. When utilized in Zn-air batteries as the cathode, it exhibits better activity, stability, and higher specific capacity than that of Pt–RuO 2 /C, showing a good potential for air cathode.
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高影响因子
ANALYTICAL CHEMISTRY
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2021
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IF 6.986
Li-Ping Zong,Junji Li,Guofang Shu,Xinye Liu,Robert S. Marks,Xue-Ji Zhang,Serge Cosnier,Dan Shan
In view of the shortcomings of the current coreactant electrochemiluminescence (ECL) and inspired by natural oxygen (O2) reduction metalloenzymes, a novel ECL amplification strategy was established. A pyrolytic iron- and nitrogen-doped (Fe–N–C) nanosheet rich in singly ionized oxygen vacancy (VO•) defects was rationally designed by destroying the highly saturated coordination with a preorganized ligand 1,10-phenanthroline-2,9-dicarboxylic acid (PDA). Extraordinary catalytic activity for O2 activation was obtained via screening a special pyrolysis temperature using spectroscopic and electrochemical methods. The high-spin ferric centers of highly dispersed FeC nanoclusters and abundant carbon and oxygen vacancy defects fully contributed to the inherent catalytic activity. ECL amplification was achieved by integrating the material with luminol to generate redox-active radicals in situ from dissolved O2 and simultaneously shorten the transferring distance of radicals. Tetracycline (TC), which posed a growing threat to aquatic biodiversity and environmental safety, as a model antibiotic was successfully detected with a detection limit of 3.88 nM (S/N = 3), clarifying a promising application prospect of this new effective ECL amplification strategy in biological analysis and environmental monitoring.
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高影响因子
Green Chemical Engineering
·
2026
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IF 11.9
Kexin Wei,Haoyang Yu,Fan Yang,Yang Sun,Shijia Li,Jiabao Guo,Yongfeng Li
To advance the development of high-performance rechargeable zinc-air batteries (ZABs) with efficient oxygen electrochemistry, significant progress is needed in research on Fe-based nanoparticle/single-atom bifunctional oxygen electrocatalysts. Nevertheless, the structure-activity relationship and synergy mechanism of Fe-based nnoparticle/single-atom hybrid catalysts are not well-known. Herein, Self-supported carbon nanofiber electrocatalysts with in-situ synthesized FeS, Fe 2 P, or Fe 3 C nanoparticles and atomically dispersed Fe-N x sites were prepared in this work by the coaxial electrospinning method. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) simulations showed that there was a significant change in charge distribution, an increase in the adsorption of *O intermediates, and a decrease in the *OH desorption energy barrier at the FeS/FeSA interface. It can be concluded that FeS/FeSA has better electronic and adsorption properties than Fe 2 P/FeSA and Fe 3 C/FeSA. Therefore, FeS/FeSA has an oxygen reduction reaction (ORR) half-wave potential of 0.89 V and an oxygen evolution reaction (OER) overpotential of 240 mV at 10 mA/cm 2 , which is relatively high compared with that of Fe 2 P/FeSA (0.79 V, 260 mV) and Fe 3 C/FeSA (0.77 V, 250 mV), and it has a small potential gap (Δ E ) of 0.58 V. FeS/FeSA can be used as the air cathode in liquid ZABs; it has a high peak power density of 116 mW/cm 2 and is stable for more than 150 hours. The above results have laid the foundation for the construction of high-performance air cathode catalysts by means of effective coupling of atomic nanoparticles and shown the direction for developing high-efficiency, long-life rechargeable zinc-air batteries.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Jinchang Xu,Yinlong Wu,Tianli He,Ruizhong Chen,Siguo He,Jian Chen,Fangyan Xie,Yanshuo Jin,Ming-Hsien Lee,Nan Wang,Zhenyou Wang,Hui Meng
Dual nitrogen-doping strategies effectively regulate both the activity and durability of Fe-N-C catalysts. • Amino-functionalized precursors generate lower-coordinated Fe N sites, leading to enhanced ORR kinetics. • Ammonia-assisted pyrolysis boosts initial PEMFC performance by modulating spin state and increasing specific surface area. • The catalytic activity and stability of PEMFCs are strongly correlated with the spin state of the Fe active sites, where high-spin configurations offer higher activity but inferior stability. Nitrogen species play a crucial role in regulating the electronic structure of Fe-N-C catalysts, thereby governing the adsorption of oxygenated intermediates and ultimately determining proton exchange membrane fuel cell (PEMFC) performance. However, the intrinsic linkage among nitrogen configuration and catalytic performance remains insufficiently understood. To address this, we design four Fe-N-C catalysts with comparable structures but distinct nitrogen components by using amino-functionalized precursors and controlling the pyrolysis atmosphere. PEMFC testing and characterization show that amino groups in the iron precursor generate lower coordinated Fe-N x site, which density functional theory calculations show to possess more favorable adsorption energetics and reduced free-energy barriers for key reaction intermediates. In contrast, ammonia-assisted pyrolysis enhances initial performance primarily by introducing higher spin-state sites, abundant carbon defects, enlarging surface area, and increasing the density of accessible Fe-N x sites. Importantly, we find that both catalytic activity and durability can be regulated by Fe-N coordination by manipulating spin state of the Fe center: high-spin sites deliver higher intrinsic activity but suffer from accelerated degradation, whereas intermediate/low-spin sites offer improved stability. These findings suggest that a rational combination of precursor functionalization and pyrolysis atmosphere can simultaneously optimize Fe-N x site spin state, coordination environment, and carbon microstructure, providing a practical strategy to achieve both high activity and long-term durability in Fe-N-C catalysts for PEMFCs. Download: Download high-res image (57KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Ting Yang,Shisuo Fan,Yang Li,Qi Zhou
A high-efficient iron-based heterogeneous catalyst is desired to active peroxymonosulfate (PMS). Due to a large catalytic contribution of atomically dispersed Fe-N x sites, single-atom iron–nitrogen-carbon catalysts exhibit superior performance in the catalytic activation of PMS. Herein, a sequence of Fe-N-C SACs with atomically dispersed Fe-N x sites, Fe SA -N-C and Fe SA -N/C, were prepared from Fe-doped ZIF-8 and FePc@ZIF-8, respectively. Single-atom Fe-N x sites were confirmed to be the main active sites for PMS activation. Fe SA -N/C-20 with a higher density of Fe-N x sites exhibited superior catalytic performance to N/C, Fe SA -N-C, Fe SA -N/C-15, and Fe SA -N/C-25 for BPA degradation. Integrated with chemical quenching experiments, electron spin resonance (ESR), in-situ Raman spectra, and electrochemical analysis, a nonradical pathway was demonstrated to dominate the degradation of BPA in the PMS + Fe SA -N/C-20 system. More importantly, the nature of this nonradical pathway was found to be an electron-transfer regime instead of a high-valent iron or singlet oxygenation process. The BPA was adsorbed onto the Fe-N x site by a “donor–acceptor complex” mechanism to form a nonradical PMS* intermediate during the process. Benefiting from this mechanism, the PMS + Fe SA -N/C-20 system showed wide pH adaptation and high resistance to inorganic anions.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Wen Song,Xinyu Xiao,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
Supporting Fe catalysts on N doped carbon (Fe-N-C) renders a promising way towards peroxymonosulfate (PMS) activation for water decontamination , but constructing high-efficiency Fe-N-C remains challenging due to the insufficient understanding of the structure-performance relationship. Herein, the N doped carbon nanotube supported Fe catalysts (Fe-NCNT) were prepared towards PMS activation for organic pollutants removal, in which the Fe-N coordination number and Fe species were tuned through changing the pyrolysis temperature to study their roles in PMS activation. Results showed increasing the pyrolysis temperature converted the Fe-N 4 structure in Fe-NCNT to low-coordinated Fe-N 3 structure and produced Fe nanoparticles (FeNP, encapsulated in carbon). The Fe-NCNT with Fe-N 3 and FeNP exhibited a remarkably high specific activity (0.119 L min −1 m −2 ), which was 1.8 times higher than that of Fe-NCNT with only Fe-N 4 and obviously outperformed those of the state-of-the-art PMS activators. The low-coordinated structure and FeNP promoted the PMS reduction on Fe 2+ of Fe-N x for •OH and SO 4 •− production, which served as major oxidants for pollutants degradation . The experimental results and theoretical calculation corroborated the low-coordinated structure and FeNP jointly enhanced the PMS adsorption and electron density on Fe center, which accelerated electron transfer from Fe center to PMS for radical production.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Lu Zheng,Yifan Gu,Fengting Li
The rational design of transition metal and nitrogen co-doped carbon-based catalysts for the efficient removal of antibiotics through non-radical pathway of peroxymonosulfate (PMS) activation has attracted widespread attention. Herein, a magnetic hierarchical porous Fe-N-C catalyst (FeBDC-NH 2 -800) was successfully constructed by pyrolyzing the hierarchical porous precursor metal–organic framework gel (FeBDC-NH 2 ) consisting of nitrogen-containing ligands. Benefiting from the defective heterojunction structure, the catalyst exhibited effective and efficient degradation towards amoxicillin (AMX) by activating PMS to produce 1 O 2 . The degradation of AMX was up to 97.4 % within 30 min, which was 2.48 and 2.16 times more than that of FeBDC-NH 2 /PMS and nanosized Fe 3 O 4 /PMS respectively. The high degradation performance could be maintained toward low pollutant concentration conditions and cycle experiments, manifesting its possibility for practical application. Combining the data of quenching experiments, electron spin resonance spectra, electrochemical experiments, X-ray photoelectron spectra and density functional theory calculation, the mechanism was revealed that radical pathway contributed little during degradation while singlet oxygen played a significant role. The cleavage of lattice oxygen and defective heterogeneous structure of FeBDC-NH 2 -800 contributed together to promote PMS for 1 O 2 production.
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危险品化学品经营许可证（带存储）