ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Yudong Zhang,Yuan He,Jun Li,Yang Xu,Yang Yang,Yao Ge,Xun Zhu,Qiang Liao
Optimizing non-noble catalysts for the oxygen reduction reaction (ORR) is crucial for advancing energy storage and conversion technologies. This study investigates the influence of iron valence states and nitrogen precursor contents on the physicochemical properties and electrochemical performance of lignin-based Fe–N–C catalysts. Catalysts are synthesized using different valence iron sources and varying pyrrole contents. The results reveal that iron(II) doping increases microporosity and specific surface area, while iron(III) doping enhances mesoporous and iron contents of the carbon materials. XPS and Raman spectroscopy confirm the successful incorporation of Fe–Nx active sites in the as-prepared LFeIIIPx catalysts. Electrochemical tests demonstrate that LFeIIIP10 exhibits the highest ORR activity, surpassing commercial Pt/C in half-wave potential (E1/2) and limiting current density (JL). The direct formate fuel cell (DFFC) with an LFeIIIP10 air cathode achieves a maximum power density of 24.7 mW cm–2, 32% higher than that with a Pt/C cathode. This study highlights the critical role of tailoring iron valence states and nitrogen levels to develop high ORR performance, cost-effective Fe–N–C catalysts, providing valuable insights for the future design of non-noble metal catalysts in energy applications.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Weikang Zhu,Yabiao Pei,John C. Douglin,Junfeng Zhang,Haoyang Zhao,Jiandang Xue,Qingfa Wang,Ran Li,Yanzhou Qin,Yan Yin,Dario R. Dekel,Michael D. Guiver
Recently, much work has been devoted to designing catalysts with high porosity and efficient active sites. Although very promising results are achieved using Co/Fe–N–C catalysts based on rotating disk electrode (RDE) tests, actual fuel cell performance is below expectations, probably due to insufficient understanding of the catalyst layer (CL). Therefore, catalyst design should be considered holistically by taking into account CL performance, not only intrinsic activity. Here, Co/Fe–N–C with highly dispersed CoFe nanoalloy in the carbon network is obtained by careful design of Co/Fe-ZIF precursor, resulting in a high oxygen reduction reaction (ORR) site density with good stability. Concerning RDE test in the kinetic region and single cell test (SCT) with complex influence factors, the half-cell test (HCT) is introduced to more accurately evaluate the quality of the Co/Fe–CL. Multi-scale measurements (RDE, HCT and SCT) in different current density ranges allows targeting the key CL influence factors for fuel cell performance.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2026
·
IF 7.9
Pengfei Wang,Chuanhui Geng,Li Shao,Mei Liu,Qian Li,Kecun Ma,Zhi Chen,Qingguo Chen
Water pollution has been worsened by increasing human activities, involving both water-soluble and non-water-soluble contaminants. In this study, a Fe-N-C@ZnO activated PS-AOP (persulfate advanced oxidation process) system was developed through the combination of photocatalysis and PS (persulfate) activation for pollutant degradation in freshwater and seawater. First, the optimal performance was determined by adjusting the Fe-N-C@ZnO to PS ratio, with the best results achieved at 5:3. The degradation efficiency and mechanisms were then examined across different pollutant types. Higher degradation rates were observed in the Fe-N-C@ZnO activated PS-AOP system compared to PS alone, in freshwater, improvements of 70.87%, 61.63%, and 46.26% were recorded for enrofloxacin (ENR), naphthalene, and crude oil, respectively. And in seawater, the increases were 57.53%, 46.87%, and 31.49%. Through radical quenching experiments, h⁺, e⁻, and SO 4 ·⁻ were identified as the dominant reactive species. Additionally, DI-MS analysis was used to propose four degradation pathways for ENR (three Piperazine-Routes and one Quinolone-Route) and two pathways for naphthalene (Benzene ring hydroxylation and Tautomerization). Download: Download high-res image (198KB) Download: Download full-size image
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14793-14805
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IF 12.732
Yuan Gao,Xiaoguang Duan,Bin Li,Qianqian Jia,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Shaobin Wang,Wenchao Peng
Persulfate-based advanced oxidation processes are promising technologies to solve water pollution. In this work, single iron atoms are anchored on three-dimensional N-doped carbon nanosheets by a chemical vapor deposition (CVD) method with ferrocene-loaded CaO as the hard template. The high surface density of Fe–N4 sites and abundant interconnected meso–macro pores are highly favorable for activating peroxymonosulfate (PMS) to produce superoxide radicals (O2˙−), giving rise to ultrahigh activity and excellent stability for pollutant degradation. Experiment and density functional theory (DFT) calculations reveal that Fe–N4 is the main active site, on which electrons transfer from C to Fe via the C–N–Fe bond to secure the low-valence state of Fe species for the redox process. This work proposes a new strategy for developing highly active single-atom materials by CVD and reveals mechanisms of PMS activation on single-atom activators.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 19
·11792-11801
·
IF 10.733
Xiang Ao,Wei Zhang,Zhishan Li,Lin Lv,Yunjun Ruan,Hong-Hui Wu,Wei-Hung Chiang,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
The scarcity and weak durability of precious metal catalysts are among the biggest obstacles to achieving cost-effective electrocatalysts in fuel cells and metal–air batteries. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to precious metal catalysts. Herein, we report a highly effective strategy for the facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 °C, and co-exist with numerous in situ formed Fe–N4 moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts exhibit high ORR activity, comparable/superior to that of the state-of-the-art Fe/N–carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V (vs. RHE) and a limited current density of 6.18 mA cm−2. By resorting to experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe–N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting the catalytic performance of the Fe/N-functionalized porous carbon networks.
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Materials
·
2020
·Vol. 13
·期 20
·4551
·
IF 3.057
Linglei Jin,Baikang Zhu,Xuesong Wang,Le Zhang,Debin Song,Jian Guo,Hengcong Tao
With the assistance of surfactant, Fe nanoparticles are supported ong-C3N4nanosheets by a simple one-step calcination strategy. Meanwhile, a layer of amorphous carbon is coated on the surface of Fe nanoparticles during calcination. Transmission electron microscopy (TEM), scanning electron microscope (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) were used to characterize the morphology, structure, and composition of the catalysts. By electrochemical evaluate methods, such as linear sweep voltammetry (LSV) and cyclic voltammetry (CV), it can be found that Fe25-N-C-800 (calcinated in 800 °C, Fe loading content is 5.35 wt.%) exhibits excellent oxygen reduction reaction (ORR) activity and selectivity. In 0.1 M KOH (potassium hydroxide solution), compared with the 20 wt.% Pt/C, Fe25-N-C-800 performs larger onset potential (0.925 V versus the reversible hydrogen electrode (RHE)) and half-wave potential (0.864 V vs. RHE) and limits current density (2.90 mA cm−2, at 400 rpm). In 0.1 M HClO4, it also exhibits comparable activity. Furthermore, the Fe25-N-C-800 displays more excellent stability and methanol tolerance than Pt/C. Therefore, due to convenience synthesis strategy and excellent catalytic activity, the Fe25-N-C-800 will adapt to a suitable candidate for non-noble metal ORR catalyst in fuel cells.Keywords:oxygen reduction reaction;iron;coating;P-123
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Taotao Lv,Mengran Lou,Chunmei Xu,Yang Wang,Ruiying Wang,Hongtao Liu,Rui Liu,Xia Kong
The Cu/Fe-N@PCFs catalyst is prepared by electrospinning and pyrolysis. • Cu active species synergize with Fe-N@PCFs to boost the catalytic performance. • Cu/Fe-N@PCFs shows excellent ORR/OER activity with a low ΔE of 0.73 V. • Flexible Cu/Fe-N@PCFs achieves high peak power densities in ZAB and FZAB. The key to advancing Zn-air batteries (ZABs) and flexible Zn-air batteries (FZABs) lies in creating electrocatalysts with flexibility, porosity, high efficiency, and stability. Herein, Cu/Fe-N@PCFs is prepared by electrospinning and pyrolysis. Fe-ZIF-8 serves as a carbon and nitrogen source dispersing Fe sites, and promotes the formation of microporous structures during pyrolysis together with NaCl. Cu species are introduced onto the surface of Fe-N@PCFs to interact with Fe-N x sites and alleviate the Fenton-like effect, synergistically enhancing the bifunctional oxygen electrocatalytic performance toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The fibrous structure improves the peak power density of ZAB and FZAB. The Cu/Fe-N@PCFs exhibits an ORR half-wave potential (E 1/2 ) of 0.865 V (vs. 0.838 V for Pt/C) and an OER overpotential of 370 mV (vs. 305 mV for RuO 2 ) at 10 mA cm −2 . The ZAB achieves a peak power density of 278.2 mW cm −2 (vs. 145.5 mW cm −2 for Pt/C + RuO 2 ) and durability of 190 h. The self-supporting Cu/Fe-N@PCFs is assembled as FZAB, delivering a peak power density of 82.4 mW cm −2 (vs. 16.4 mW cm −2 for Pt/C + RuO 2 ) and durability of 17 h. This study provides significant perspectives on constructing flexible catalysts, potentially advancing the development of ZABs and FZABs. Download: Download high-res image (266KB) Download: Download full-size image
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FUEL PROCESSING TECHNOLOGY
·
2022
·
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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
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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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.
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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 .
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