ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Liping Sun,Chao Li,Yong Yan,Yue Yu,Hao Zhao,Zijue Zhou,Feng Wang,Yi Feng
Single atom nanozymes (SAzymes) represent the state-of-the-art technology in nanomaterial-based catalysis, which have attracted attentions in catalysis, cancer treatment, disinfection and biosensing fields. However, numerous SAzymes suffered from low aqueous dispersion and without recognition capacity, which impeded their applications in bioanalysis . Herein, we engineered DNA onto SAzymes to obtain the DNA/SAzymes conjugates , which significantly improved the aqueous dispersion and recognition ability of SAzymes. We synthesized iron SAzymes (Fe–N–C SAzymes) as the catalytic nanomaterials, and investigated the interactions between Fe–N–C SAzymes and DNA. We compared A 15 , T 15 and C 15 adsorption of Fe–N–C SAzymes in HEPES containing 2 mM MgCl 2 . We found that 50 μg mL −1 Fe–N–C SAzymes produced nearly 100% A 15 adsorption, 90% T 15 adsorption and only 69% C 15 adsorption, indicating that adenine and thymine had higher adsorption affinity on Fe–N–C SAzymes. More importantly, DNA modification did not affect the peroxidase-like activity of Fe–N–C SAzymes and the bioactivity of the adsorbed DNA. Taking the advantage of the diblock DNA with one DNA sequence (adenine) binding to Fe–N–C SAzymes and the other DNA sequence (i.e., aptamer) binding to cancer cells, we designed Apt/Fe–N–C SAzymes for colorimetric detection of cancer cells, which offered new insights for the use of SAzymes in biomedicine .
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Mengxue Li,Juanjuan Wang,Nana Zhu,Yang Zong,Rui Jiao,Zhaoqi Zhu,Hanxue Sun,An Li
Fe–N–C catalysts are some of the most promising catalysts for the oxygen reduction reaction (ORR). However, there are still some problems in the pyrolysis of precursors, such as the destruction of the carbon skeleton and low utilization of active sites. In this work, we synthesized hollow pyridine N-containing conjugated microporous polymers (CMPs) by coupling polymerization. The bipyridine units in CMPs’ skeleton can anchor Fe3+ to form a stable coordination structure, which was effectively converted into Fe–N–C catalysts by one-step pyrolysis. Due to the rigid skeleton of precursors, the hollow structure was preserved in catalysts, which is favorable to O2 diffusion and mass transport of intermediates. X-ray photoelectron spectroscopy and Fe K-edge X-ray near-edge spectroscopy revealed approximate FeN4 structures within the framework of the catalysts. As a result, the resulting CMP-derived catalysts exhibited satisfactory ORR activity in alkaline media with a limiting current density of 4.40 mA cm–2. Furthermore, the Fe,N–C1–900 catalyst demonstrated exceptional methanol immunity with a mere negative shift of 0.01 mA cm–2 in limiting current density compared with the commercial Pt/C catalyst, indicating remarkable stability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Youyou Feng,Jing Qin,Yu Zhou,Qin Yue,Jing Wei
Nanozyme has been regarded as an efficient antibiotic to kill bacteria using the reactive oxygen species (ROS) generated by Fenton-like reaction. However, its activity is still unsatisfied and requires large amount of hydrogen peroxide with side effects toward normal tissues. Herein, spherical mesoporous Fe-N-C single-atom nanozyme (SAzyme) is designed for antibacterial therapy via photothermal treatment enhanced Fenton-like catalysis process. Due to the large pore size (4.0 nm), high specific surface area (413.9 m 2 g −1 ) and uniform diameter (100 nm), the catalytic performance of Fe-N-C SAzyme is greatly improved. The Michaelis-Menten constant ( K m ) is 4.84 mmol L −1 , which is similar with that of horseradish peroxidase (3.7 mmol L −1 ). Moreover, mesoporous Fe-N-C SAzyme shows high photothermal conversion efficiency (23.3 %) owing to the carbon framework. The catalytic activity can be enhanced under light irradiation due to the elevated reaction temperature. The bacteria can also be killed via physical heat effect. Due to the synergistic effect of nanozyme catalysis and photothermal treatment, the antibacterial performance is much higher than that using single antibacterial method. This work provides an alternative for combined antibacterial treatment via photothermal treatment assisted catalytic process using spherical mesoporous single-atom nanozyme as an antibiotic.
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高影响因子
NANOTECHNOLOGY
·
2019
·Vol. 30
·期 30
·305402
·
IF 3.399
Tong Wu,Yaying Li,Yuntong Li,Jing Hong,Haiyang Wu,Jie Mao,Yuzhe Wu,Qipeng Cai,Conghui Yuan,Lizong Dai
Simultaneous introduction of both transition metal and other inorganic elements into the carbon matrix has attracted great attention in the fabrication of carbon materials with high electrochemical properties. Herein, rational design of ligand-iron coordinative supramolecular precursors is achieved for the fabrication of Fe-N/C catalysts, which possess high oxygen reduction reaction (ORR) performance. A series of precursors are prepared by a simple coordination reaction between a three armed catechol monomer and iron ions. Particular interest is focused on tuning the doping species, surface area and morphology of the Fe-N/C catalysts through a simple selection of iron resources. We show that an Fe-N/C catalyst derived from Fe2(SO4)3 at a carbonization temperature of 800 °C, has the optimized ORR performance with an onset potential of 0.930 V and half-wave potential of 0.801 V. Detailed investigation indicates that the synergistic effect among doping elements of nitrogen and sulfur and the unique carbon structure determines the performance of the Fe-N/C catalysts. Our findings may be of significance for the fabrication of doped carbon materials using coordinative supramolecular polymers as precursors.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 15
·7145-7157
·
IF 11.301
Jinling Xue,Yinshi Li,Jue Hu
It remains a major challenge to develop a facile method to prepare non-noble metal electrocatalysts with high activity and durability to drive the sluggish oxygen reduction reaction (ORR) for proton exchange membrane fuel cells (PEMFCs). Herein, a highly efficient bimetallic Zn/Fe@N-doped hierarchical porous carbon (Zn/Fe–N–C) catalyst derived from ZIF-8 and hemin (host–guest) was firstly reported by one-step thermal treatment. Fe2+ spatially separated by using the hemin guest in the ZIF-8 framework and hydrocarbon-branched chains form rich Fe–Nx active sites, and the evaporation of Zn2+ generates a highly porous structure in the Zn/Fe–N–C catalysts. Benefitting from this unique structure and composition, the resulting Zn/Fe2–N–C catalyst exhibits excellent ORR activities in both 0.1 M KOH (onset potential, Eonset = 1.08 V, and half-wave potential, E1/2 = 0.86 V vs. RHE) and 0.5 M H2SO4 media (Eonset = 1.04 V and E1/2 = 0.81 V), which are even comparable to those of the commercial Pt/C catalyst, and ranks among the top reported electrocatalysts. In addition, it also has outstanding long-term durability and good methanol resistance, much better than those of Pt/C in both acidic and alkaline media, which makes it one of the best non-noble alternatives of Pt-based catalysts for ORR electrocatalysis. This work highlights the potential to rationally design and fabricate high-performance ORR catalysts for fuel cell applications.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 58
·14597-14603
·
IF 5.317
Xinghua Chen,Fei He,Yanfei Shen,Yiran Yang,Hao Mei,Songqin Liu,Toshiyuki Mori,Yuanjian Zhang
Graphical Interface effect : A study into the intrinsic role of carbon supports for Fe-N/C alternatives to Pt/C catalysts for oxygen reduction in fuel cells revealed that when immobilized on suitable support, the Fe−N/C demonstrated an improved mass J K that was comparable to that of Pt/C and higher than most reported M−N/C catalysts (see scheme). The mass kinetic current density (mass J K ) of most extensively reported M−N/C catalysts (M represents non-precious metal elements such as Fe, Co, and Cu), a potential alternative to noble metal catalysts in fuel cells, is poorer than that of commercial Pt/C. Thus, deep understanding of the intrinsic roles of carbon supports may contribute to the development of M−N/C catalysts from a practical point of view. Herein, the routinely used carbon supports, i.e. carbon black (CB) and carbon nanotubes (CNT) that have different morphology and crystallinity, were investigated to uncover the factors that affected the mass J K of Fe−N/C in electrocatalytic oxygen reduction. When immobilized on CB, the ionic liquids-derived Fe−N/C exhibited an enhanced mass J K (4.45 A g −1 at 0.80 V vs. RHE) by a factor of 2.14 times, comparable to that of Pt/C (5.79 A g −1 ) and higher than most reported M−N/C catalysts to our best knowledge. In contrast, the CNT support system showed no improvement. It was revealed that a compatible interface between the Fe−N/C precursors and the carbon supports was vital to ensure in-situ growth of a uniform catalyst layer on the supports during pyrolysis. This subsequently promotes the mass J K by exposing more embedded active sites and introducing favorable slit pores for effective mass-diffusion. This work would be promising to address the long-term overlooked challenge of the low mass J K of M−N/C catalysts in replacing noble-metal catalysts for practical fuel cell applications.
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高影响因子
Nanoscale
·
2019
·Vol. 11
·期 41
·19506-19511
·
IF 6.97
Ying Li,Tong Liu,Wenxiu Yang,Zhijun Zhu,Yanling Zhai,Wenling Gu,Chengzhou Zhu
Non-Pt catalysts with excellent performance regarding the oxygen reduction reaction (ORR) have aroused enormous interest in recent years. Herein, we propose a dual-template method to synthesize a multiscale porous Fe–N–C (FeNC) catalyst. SiO2 and Zn are used as co-templates to produce a multiscale porous structure. Chitosan and glutaraldehyde are used as building blocks to fabricate the frameworks of the hydrogel. After lyophilization and annealing treatments, FeNC aerogel with a multiscale porous structure could be obtained. The as-prepared FeNC catalyst annealed at 900 °C (FeNC-900) exhibits a larger electrochemically active surface area and an improved ORR activity compared to FeNC annealed at other temperatures. FeNC-900 shows a superior ORR performance in comparison with that of commercial Pt/C in terms of the onset potential and half-wave potential, i.e., 0.959 and 0.837 V, which are 28 mV and 10 mV higher than those of Pt/C, respectively. Multiscale porosity is responsible for the outstanding ORR performance of FeNC-900. The electron transfer number of FeNC-900 for the ORR was calculated to be 3.95, which is comparable with that of Pt/C. In addition, the FeNC-900 catalyst possesses an excellent long-term duration and anti-poisoning capacity against methanol crossover. All these results endow the FeNC catalyst with tremendous potential for use in fuel cells.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2026
·Vol. 28
·期 6
·165
·
IF 3.5
Yang Menghui,Gao Zhen,Zhan Haoyu,Bi Mengqi,Huang Naibao,Zhang Junjie,Gan Ziqi,Wang Hao
Developing highly active, durable, and cost-effective oxygen reduction reaction (ORR) catalysts is crucial for fuel cell commercialization through the use of non-precious metal alternatives to platinum. In this study, the tunable dodecahedral Fe-N-C catalysts were synthesized through controlled pyrolysis of Fe-doped zeolite imidazolate framework-8 (ZIF-8) precursors. The optimized 5% Fe@NC-8 catalyst demonstrates excellent ORR performance with an onset potential of 0.92 V vs. RHE, a half-wave potential (E 1/2 ) of 0.83 V vs. RHE, and a limiting diffusion current density (j d ) of 6.06 mA cm −2 , surpassing commercial 20% Pt/C catalysts (onset potential 0.89 V vs. RHE; E 1/2 0.81 V vs. RHE; j d 4.27 mA cm −2 ). It also shows strong durability, retaining 86.16% of its current after prolonged polarization (@0.80 V vs. RHE for 10,000 s) and minimal negative shift in half-wave potential after extensive cycling(@200 mV s −1 for 5000 CV cycles). The enhanced catalytic performance is attributed to (i) possessing a high specific surface area (319 m 2 g −1 ) and favorable porosity to maximize active site accessibility; (ii) having abundant active sites of Fe-N x , graphitic N, and pyridinic N as active catalytic centers; and (iii) forming N-doped carbon matrices to provide a conductive framework. These advantages boost the density of accessible active sites and thus remarkably improve the ORR catalytic activity.
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International Journal of Electrochemical Science
·
2023
·Vol. 14
·期 6
·5820-5830
·
IF 1.5
Yao Liug,Xiaojing Liug,Junli Liu,Chaozhong Guo,Yanrong Li,Jin Zhang,Zhongbin Li
Ternary Fe-N-C catalysts are regarded as the most promising candidates for low-cost alternatives to the Pt-based materials for catalyzing the oxygen reduction reaction (ORR). In this paper, the Fe and N codoped carbon catalyst (Fe-Py@K-800) with the unique foam-like 3D structure has been fabricated by using the molecular sieve as a new solid-state template. The results of physical characterization indicate that Fe atoms are coordinated with nitrogen atoms to form the Fe-N ORR-active structure. In contrast with the commercial Pt/C catalyst, the Fe-Py@K-800 displays a comparable ORR electrocatalytic activity with an onset potential of ~1.1 V and a half-wave potential of ~0.88 V ( vs. RHE), however, the long-term stability of Fe-Py@K-800 is obviously better. These results show that iron-organic coordination in the pyrrole ring will play a role in the generation of nitrogen-rich active sites, which facilitates the enhancement of ORR activity in alkaline electrolyte.
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ADVANCED MATERIALS
·
2026
·
IF 26.8
Zhechen Fan,Shuhu Yin,Wenhao Miao,Yudie Zhou,Weiyi Zhao,Yixuan Yin,Hao Yu,Lin Lin,Lina Hou,Hao Wan,Ying Wang,Junjie Ge
Atomically dispersed Fe–N–C catalysts are regarded as promising alternatives to platinum-group-metal (PGM) catalysts for proton exchange membrane fuel cells (PEMFCs). However, their further development is hindered by inadequate utilization of active sites in membrane electrode assembly (MEA). Herein, we developed a high mass activity O–FeNC catalyst with high site density and enhanced site utilization. C═O groups function as hard base linkers, promoting the densification of FeN 4 sites through Lewis acid-base interactions. Moreover, they also direct interfacial alignment within triple-phase boundaries, leading to concentrated hydronium ions and accelerated oxygen permeation via regulated ionomer nanophase segregation. As a result, the obtained O–FeNC cathode delivered a current density of 66.45 mA cm −2 at 0.90 V iR-free , surpassing the US Department of Energy 2025 target (44 mA cm −2 at 0.9 V iR-free ), with a mass activity that is 59% higher than commercial Pt/C. The peak power densities reached 1.8 W cm −2 under H 2 –O 2 and 0.93 W cm −2 under H 2 –air, alongside demonstrated industrial scalability through gram-scale synthesis and a 500 W PGM-free cathode stack prototype.
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高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Yabiao Pei,Weikang Zhu,Runfei Yue,Jie Yao,Xin Liu,Lianqin Wang,Junfeng Zhang,Yan Yin,Michael D. Guiver
Adjusting catalyst/ionomer agglomerate is crucial to a high-performance catalyst layer (CL), particularly for non-precious metal catalysts . As a sacrificial component, the solvent plays a vital role during the CL formation process and resulting microstructure, determining the performance of the anion exchange membrane fuel cells (AEMFCs). Here, solvent mixtures of isopropanol (IPA) and tetrahydrofuran (THF) are studied for the controllable construction of the Co/Fe–N–C CL. The results indicate that the aggregate state of the ionomers and catalysts and the final CL microstructure strongly depend on the ratio of IPA and THF. The CL prepared with IPA: THF = 1:2 (v/v) shows a homogeneous distribution of Co/Fe–N–C catalysts, embedded in the ionomer matrix, due to the fast volatilization and low viscosity of the catalyst ink. The Co/Fe–N–C CL with high moisture adsorption behavior and retention ability results in a high performance AEMFC with peak power density of 545.3 mW cm −2 at 80 °C. The obtained results can guide the rational design of microstructure in non-precious metal CLs for high-performance AEMFCs.
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