CHEMICAL ENGINEERING JOURNAL
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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.
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高影响因子
ACS Applied Materials & Interfaces
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2018
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IF 8.097
Fei He,Li Mi,Yanfei Shen,Toshiyuki Mori,Songqin Liu,Yuanjian Zhang
Developing highly efficient biomimetic catalysts that directly use O2 as the terminal oxidant to dehydrogenate and monoxygenate substrates with high selectivity under mild conditions has long been pursued but rarely achieved yet. Herein, we report that heterogeneous Fe–N–C, which is commonly used as an electrocatalyst for oxygen reduction reaction, had unusual biomimetic catalytic activity in both dehydrogenation and monoxygenation of a series of organic molecules (∼100% selectivity) by directly using O2. The Fe–Nx center was verified to be the active site that reductively activated O2 by spontaneously generating specific reactive oxygen species (ROS) (1O2, O2•–, and H2O2). Aided by these ROS, under physiological conditions, the Fe–N–C was further successfully exampled to kill proliferative lung cancer cells. Fe–N–C had several striking superior features with respect to natural enzymes, classical heterogeneous nanozymes, and homogeneous artificial enzymes incapable of working under harsh conditions (extreme pH and high temperature), ease of separation and recycling, and direct use of O2. It would open up a new vista of Fe–N–C as an artificial enzyme in biomimetic catalysis, ranging from fundamental simulation of oxidase/oxygenase metabolism to industrial oxidation processes and to disease treatment.
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PubMed
高影响因子
Nanoscale
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2024
·Vol. 16
·期 48
·22273-22282
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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.
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ACS Applied Materials & Interfaces
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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
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2021
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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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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Yuzhe Liu,Qi Li,Yuhan Liang,Junhao Liang,Wenliang Feng,Bin Wu,XuLei Sui,Zhenbo Wang
The inherently low active site accessibility of single-atom Fe-N-C catalysts severely compromises their catalytic activity relative to Pt-based catalysts, thereby hindering their practical implementation in critical applications. This work systematically investigates the synergistic effects of physical confinement and chemical induced growth strategy on optimizing active site accessibility of Fe-N-C catalysts for oxygen reduction reaction. Through a physical confinement strategy, the catalyst particle size is successfully reduced from the micrometer scale to the nanometer scale. Subsequently, by employing chemical-induced growth, the particle size is precisely controlled within the range of 623 nm to 421 nm, simultaneously establishing an optimal balance between the catalyst particle size threshold (420 nm) and the ordered macroporous framework. This approach maximized the accessibility of active sites and significantly enhanced the catalytic activity of the Fe-N-C catalyst. The optimized catalyst (OM-Fe-NC-4) exhibits outstanding performance, achieving a remarkable half-wave potential of 0.888 V, surpassing both commercial Pt/C and most state-of-the-art Fe-N-C catalysts. Additionally, it demonstrates excellent four-electron selectivity and delivers a kinetic current density of 14.7 mA cm −2 at 0.85 V in acidic medium. This dual-dimensional modulation strategy offers a paradigm for enhancing the accessibility of active sites for non-precious metal catalysts.
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高影响因子
Science Advances
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2022
·Vol. 8
·期 44
·
IF 14.957
Yu-Cheng Wang,Wen Huang,Li-Yang Wan,Jian Yang,Rong-Jie Xie,Yan-Ping Zheng,Yuan-Zhi Tan,Yue-Sheng Wang,Karim Zaghib,Li-Rong Zheng,Shu-Hui Sun,Zhi-You Zhou,Shi-Gang Sun
The rational design of non-Pt oxygen reduction reaction (ORR) catalysts and catalyst layers in fuel cells is largely impeded by insufficient knowledge of triple-phase boundaries (TPBs) in the micropore and mesopore ranges. Here, we developed a size-sensitive molecular probe method to resolve the TPB of Fe/N/C catalyst layers in these size ranges. More than 70% of the ORR activity was found to be contributed by the 0.8- to 2.0-nanometer micropores of Fe/N/C catalysts, even at a low micropore area fraction of 29%. Acid-alkaline interactions at the catalyst-polyelectrolyte interface deactivate the active sites in mesopores and macropores, resulting in inactive TPBs, leaving micropores without the interaction as the active TPBs. The concept of active and inactive TPBs provides a previously unidentified design principle for non-Pt catalyst and catalyst layers in fuel cells.
研究领域:
燃料电池
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催化
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材料科学
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电化学
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纳米技术
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高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2026
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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
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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
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2019
·Vol. 7
·期 19
·11792-11801
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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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高影响因子
APPLIED SURFACE SCIENCE
·
2026
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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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