ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
DanDan Yang,Jingqi Chen,Yuting Huang,Ganghui Chen,Xueliang Liu,Xuan Wang,Like Yang,Zhaohui Li,Jie Hu,Qi Zhou,Jia Ge,Yu Yang
The development of cost-effective and easy-to-use strategies for the detection of ascorbic acid (AA) and acid phosphatase (ACP) is in high demand but challenging. Thus, we report a novel colorimetric platform based on Fe–N/C single atom nanozyme with efficient oxidase mimicking activity for their highly sensitive detection . The designed Fe–N/C single atom nanozyme can directly oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to produce a blue oxidation product (oxTMB) in the absence of H 2 O 2 . In addition, L-ascorbic acid 2-phosphate can be hydrolyzed to ascorbic acid in the presence of ACP, which inhibits the oxidation reaction and results in a significant bleaching of the blue color. Based on these phenomena, a novel colorimetric assay with high catalytic activity was developed for the determination of ascorbic acid and acid phosphatase with detection limits of 0.092 μM and 0.048 U/L, respectively. Notably, this strategy was successfully applied to the determination of ACP in human serum samples and evaluate ACP inhibitors, indicating its potential as a valuable tool for clinical diagnosis and research.
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PubMed
高影响因子
ChemPlusChem
·
2022
·Vol. 87
·期 10
·e202200312
·
IF 3.21
Yujun Wang,Rongxiu Tu,Chuantao Hou,Zonghua Wang
Graphical A porous Fe−N−C aerogel catalyst was synthesized by pyrolysis of porous metal-organic aerogels. The Fe−N−C aerogel shows enhanced catalytic performance for oxygen reduction reaction (ORR) under alkaline condition. The markedly enhanced ORR performance for Fe−N−C aerogel can be assigned to the synergistic catalytic effect between Fe−N catalytic sites and graphitized carbon and excellent mass transport due to the unique hierarchically porous architecture. Synthesis of Fe−N−C electrocatalysts by pyrolysis of porous materials has been shown to be a promising pathway for the oxygen reduction reaction (ORR). Metal-organic aerogels (MOAs) with unique micropores and mesopores should provide an excellent precursor for Fe−N−C electrocatalysts. This work reports a Fe−N−C aerogel synthesized by pyrolysis of MOA. The Fe−N−C aerogel shows excellent ORR performance in alkaline condition with an onset potential of 0.96 V (vs. RHE) and a limiting current density of 5.02 mA cm −2 . The markedly enhanced ORR performance for Fe−N−C aerogel can be assigned to the synergistic catalytic effect between Fe−N catalytic sites and graphitized carbon and excellent mass transport due to the unique hierarchically porous architecture. In addition, satisfactory durability and methanol tolerance were obtained, demonstrating a promising material for ORR.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Zhiwen Gan,Tian Zhang,Xuanxuan An,Qin Tan,Shujun Zhen,Xiaoli Hu
Numerous ratiometric fluorescence nanozyme sensors are developed, though, fluorescence-scattering ratiometric sensors based on nanozymes are hardly reported. First-order scattering (FOS) could be quenched due to inner filter effect of quenchers on scattering signals. Meanwhile, Second-order scattering (SOS) depended on FOS. Based on the principle, we designed a novel nanozyme sensor by coupling fluorescence (FL) and SOS. Specifically, Fe-N-C nanozyme (Fe-HCNP) was fabricated by doping Fe into carbon-nitrogen polymers via formamide condensations . Fe-HCNP possessed robust oxidase-like activity, effectively transforming O 2 into ·O 2 - and ·OH. Then, Fe-HCNP and o-phenylenediamine (OPD) severed as a hybrid system to construct an FL-SOS ratiometric sensor for ascorbic acid (AA). Fe-HCNP with large size possessed strong SOS. After being added into the Fe-HCNP/OPD system, AA could fast be oxidized to dehydroascorbic acid (DAA) due to Fe-HCNP as oxidase mimics. Subsequently, fluorescent quinoxaline derivative (DFQ) was produced after condensation reactions between DAA and OPD, causing an increase in fluorescence. Meanwhile, the intensity of FOS was reduced because FOS peaks of Fe-HCNP overlapped absorption bands of DFQ, causing a decrease in SOS. The FL-SOS ratiometric sensor for AA showed outstanding advantages of high specificity and fast. Overall, this work provided a new strategy for nanozyme ratiometric sensors.
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RSC Advances
·
2022
·Vol. 12
·期 16
·9543-9549
·
IF 4.036
Tanlun Wang,Chenxiang Sun,Yong Yan,Fan Li
Metal–N–C-based catalysts prepared by pyrolysis are frequently used in the oxygen reduction reaction (ORR). Zeolitic imidazolate frameworks (ZIFs), a type of metal organic framework (MOF), are selected as precursors due to their special structure and proper pore sizes. A series of Fe–N–C catalysts with different concentrations of 2-methylimidazole were prepared with a simple solvothermal-pyrolysis method, and the transformation productivity, morphology and ORR activity were investigated. It was found that the Fe–N–C catalyst with a 2-methylimidazole concentration of 0.53 mol L−1 had the best performance. In 0.1 M KOH solution, the half-wave potential was 0.852 V (vs. RHE), with the highest electrochemically active surface area (ECSA) of 94.1 cm2, and the ORR reaction was dominated by a 4-electron process. The current only decreased by 10.5% after 50 000 s of chronoamperometry (CA), while the half-wave potential only decreased 20 mV in 3 M methanol. Additionally, this catalyst cannot be poisoned by Cl− and SO32− ions in the ORR process. Finally, some typical ions including SCN−, Fe(CN)63− and Fe(CN)64− were used to inhibit the active sites, and it was determined that Fe(II) is the real active species. The series of synthesis and testing experiments has significance in guiding optimization of the synthesis conditions and analysis of the mechanism of active sites in Fe–N–C materials.
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ChemCatChem
·
2021
·Vol. 13
·期 11
·2683-2690
·
IF 5.686
Xinxin Jin,Yan Xie,Junhong Fu,Chaoyue Zhao,Yinghao Xu,Yang Lv,Bingsen Zhang,Keju Sun,Rui Si,Jiahui Huang
Graphical ORR : We fabricated a FeSA/HNPC electrocatalyst with well atomically dispersed FeN 4 species. DFT calculations uncovered that the single-atomic FeN 4 sites within FeSA/HNPC electrocatalyst present in the configurations of pyrrole-N 4 −Fe are more favorable than those of pyridine-N 4 −Fe for boosting ORR performances. Atomically dispersed Fe−N−C electrocatalysts have displayed excellent catalytic performances towards the oxygen reduction reaction (ORR), while the identification of the genuine active sites remains a challenge. Herein, we report a Fe−N−C electrocatalyst of FeSA/HNPC featuring single-atomic FeN 4 sites on hierarchically N-doped porous carbon (HNPC), which shows a very competitive ORR activity in alkaline solution even at a low electrocatalyst loading of 0.2 mg cm −2 on the working electrode. A comparison of energy barriers in ORR reveals that the single-atomic FeN 4 active sites in FeSA/HNPC existing in the form of pyrrole-N 4 −Fe is more favorable than that of pyridine-N 4 −Fe for the enhanced ORR activity. Understanding the nature of FeN 4 active sites will greatly benefit the design of Fe−N−C electrocatalysts with highly effective ORR performances.
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CHINESE CHEMICAL LETTERS
·
2021
·
IF 6.779
Min Zhang,Bolong Yang,Ting Yang,Yahui Yang,Zhonghua Xiang
Unremitting and intensive researches about efficient non-precious metal electrocatalysts are necessary for large-scale commercial applications of fuel cells, while iron and nitrogen co-doped carbon (Fe-N-C) materials has become one of the most promising electrocatalysts to replace Pt-based noble metal catalysts . However, the traditional Fe-doped ZIF with rhomb dodecahedron morphology limits the exposure of active sites and the utilization of atoms, even affecting the performance of the catalyst. Herein, a Fe/N co-doped catalyst with a flower-like morphology was prepared using ferric citrate source along with secondary NH 3 heat treatment. The optimal catalyst (termed as 4Fe citrate -N-C-3) showed distinguished oxygen reduction reaction (ORR) activity with a half-wave potential of 0.8 and 0.9 V ( vs . RHE) in acid and alkaline media, respectively. In addition, 4Fe citrate -N-C-3 maintained more than 80% of original activity even after 50,000 s which is superior to the benchmark Pt/C. The strategy of controlling morphology and composition is meaningful for the optimization of non-precious metal electrocatalysts for ORR in fuel cells or metal-air batteries .
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xingyu Zhong,Jianing Li,Weiyu Fang,Yuxuan Shen,Mei Bai,Xiulan Hu
The advancement of high-performance oxygen reduction reaction (ORR) catalysts is increasingly responsible for energy development. Iron and nitrogen co-doped carbon materials (Fe-N-C) have garnered extensive attention because of their catalytic activity, which is comparable to that of precious metal-containing catalysts. Nevertheless, the precursor ZIF-8 inevitably forms clusters during the conventional pyrolysis preparation procedure, leading to the coverage of Fe-N active sites and inhibiting catalytic performance. In this study, we induced ZIF-8 to deform into a unique interpenetration twin structure (ZIF-8-IT) by introducing the surfactant cetyltrimethylammonium bromide (CTAB), it has a concave-convex morphology with abundant facets that enhanced interfacial contactability, thereby reducing particle-to-particle interactions and alleviating agglomeration during pyrolysis. The Fe-N-C-IT catalyst prepared using ZIF-8-IT as a precursor exhibited exceptional ORR performance in alkaline media (E 1/2 = 0.898 V, E 0 = 0.983 V). Furthermore, the Fe-N-C-IT based coulomb electrolytic oxygen sensor demonstrated superior performance compared to Pt/C, it achieved an average response time of 66 s within the 100–1000 ppm oxygen concentration range, with only a 4.9 % current fluctuation observed after 28 days at a concentration of 500 ppm oxygen. This study presents a novel strategy for developing efficient oxygen reduction electrocatalysts through morphology engineering.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·062501
·
IF 4.386
Chanez Maouche,Yazhou Zhou,Bing Li,Chao Cheng,Zirui Wu,Xue Han,Shaosheng Rao,Yi Li,Nasir Rahman,Juan Yang
Iron-nitrogen-carbon graphitic (Fe-N-C), a noble metal-free catalyst holds a lot of promise to substitute platinum (Pt) as an efficient catalyst in the oxygen reduction reaction (ORR). However, the synthesis process and the stabilization of single atoms that tend to aggregate, without jeopardizing the catalytic activity remain challenging. Here we demonstrate a stabilized assisted method for the preparation of Fe-N-C electrocatalyst by using graphitic carbon nitride (g-C3N4) nanosheet as a template. Fe ions are absorbed on the surface of g-C3N4 and imprisoned after the addition of pyrrole, preventing Fe migration that may result in nanoparticles. During the pyrolysis, Fe atoms coordinated with N provided by g-C3N4 and pyrrole on graphitic carbon to form Fe-N-C with a metal loading of 5.4 wt%. Moreover, FeNx species were introduced in the graphitic carbon, where the coexistence of micro and mesopores were favorable to offer a larger density of active sites compared to Fe/NP without pyrrole. Fe-N-C demonstrated a good electrocatalytic performance with a half-wave potential (E1/2) of 0.82 V (vs reversible hydrogen electrode (RHE)) higher than Fe/NP (0.76 V) and close to Pt/C, with a superior long stability of 85% in alkaline media after 40000 s.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yuzhe Liu,Qi Li,Yuhan Liang,Junhao Liang,XuLei Sui,Zhenbo Wang
The non-precious metal Fe-N-C catalyst is regarded as a potential substitute for the precious metal catalysts for the oxygen reduction reaction (ORR) application. However, its catalytic activity and stability still fall short of those of the precious metal catalysts. Here, Fe-N-C catalyst with an ordered macroporous framework was achieved through using polystyrene (PS) as templates. The results indicate the particle size and structural orderliness of PS templates have great influence on the morphology and the catalytic performance of the obtained Fe-N-C catalysts. The optimized catalyst, derived from ordered PS with 200 nm, exhibits exceptional ORR activity in acidic media with a half-wave potential of 0.885 V (vs. RHE), surpassing commercial Pt/C (0.847 V) and Fe-N-C without PS counterparts (0.796 V), and superior mass activity (26.54 A g⁻¹, 0.8 V) and kinetic current density (14.7 mA cm⁻²,0.85 V), while maintaining outstanding durability under 30,000 potential cycles (18 mV loss). The catalyst, as the cathode in an H₂/O₂ fuel cell, exhibits a peak power density of 0.83 W cm⁻². This excellent activity arises from its regular morphology combined with ordered macroporous framework facilitating active site exposure and reactant diffusion. The regularly arranged template-induced structural ordering enhances the graphitization and integrity of carbon matrix during pyrolysis, promoting the stability. These findings establish a template-size-dependent design principle for non-precious metal catalysts, offering a viable pathway to balance activity-stability trade-offs in proton-exchange membrane fuel cells and related electrochemical energy technologies.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yifan Zhang,Sylvestre Ndayiragije,Ming Chen,Xiaobo Wang,Lihua Zhu,Nan Wang
Fe- and nitrogen-doped carbonaceous (Fe-N-C) sites supported on MnO 2 (Fe-N-C@MnO 2 ) were prepared by a solvent-free mechanochemical method for peroxymonosulfate (PMS) activation to degrade norfloxacin (NFX). After a 50-min ball milling of iron(II) phthalocyanine (Fe( II )Pc) and MnO 2 at a weight ratio of 7.5 %, the obtained Fe-N-C@MnO 2 exhibited exceptional activity in PMS activation, achieving nearly complete degradation of NFX in 5 min with a rate constant of 0.62 min −1 . This rate constant was 11.5 and 28.2 times higher than that for milled MnO 2 (bm-MnO 2 ) and the mixture of Fe( II )Pc and MnO 2 , respectively. Alternative iron sources (FeSO 4 , FeCl 2 , Fe(III)-EDTA) and phthalocyanine showed no enhancement. Characterization revealed Fe-N-C@MnO 2 possessed abundant Mn 3+ , oxygen vacancies and Fe-N-C sites. Combined experimental and computational studies demonstrated Fe-N-C@MnO 2 simultaneously enhanced the 1 O 2 generation and facilitated the formation of SO 4 •− , •OH and O 2 •− , with contributions to NFX degradation following: 1 O 2 > •OH ≈ O 2 •− > SO 4 •− . This work establishes mechanochemical coordination engineering as a facile strategy for constructing high-performance metal-N-C hybrid catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yangyang Liu,Fengdi Tu,Ziyu Zhang,Zigang Zhao,Pan Guo,Lixiao Shen,Yunlong Zhang,Lei Zhao,Guangjie Shao,Zhenbo Wang
Iron and nitrogen co-doped carbon (Fe/N/C) electrocatalysts have great potential to catalyze the kinetically slow oxygen reduction reaction (ORR). Unfortunately, the ORR performance of existing Fe/N/C catalysts is seriously hindered by the insufficient density and accessibility of the atomic Fe-N x moieties. Herein, the carboxylate (OAc) molecular scissor is proposed to tailor Fe doped zeolitic-imidazolate-framework-8 (ZIF-8) at atomic scale and construct a multi-dimensional concave Fe@NC catalyst structure (Fe@MNC-OAc). This molecular scissoring strategy imparts Fe@MNC-OAc with dense accessible active sites, multidimensional mass transfer pathways, hierarchical porous structure, and entangled carbon nanotubes network. Therefore, the tailored Fe@MNC-OAc electrocatalyst exhibits excellent ORR activity in acidic media with a half-wave potential of 0.838 V, which is comparable to state-of-the-art non-precious metal catalysts. When assembled as cathode catalyst in a H 2 -O 2 proton exchange membrane fuel cell, it delivers a peak power density of 903 mW cm −2 . This work provides a new approach to tailoring the catalyst architecture and improving the accessibility of active sites.
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高影响因子
JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Ruite Gu,Tingyu Yan,Zeyu Hao,Huanlu Tu,Shansheng Yu,Xiaoying Hu,Hongwei Tian
The preparation of highly efficient, stable, and cost-effective catalysts to address the complex oxygen reduction reaction (ORR) in zinc-air batteries remains a significant challenge. Herein, a surface modification strategy is employed to uniformly encapsulate an Fe-N-C matrix with cobalt-coordinated conjugated organic polymers containing Schiff base structures, successfully yielding a highly active CB(cobalt-coordinated Schiff-base polymer)@Fe-N-C composite catalyst with coexisting cobalt coordination polymers and iron-nitrogen-carbon structures. In alkaline electrolytes, the CB@Fe-N-C catalyst exhibits outstanding catalytic activity (E 1/2 = 0.93 V) and stability, which are attributed to its highly conductive, structurally stable composite architecture with abundant active sites. In a zinc-air battery (ZAB), CB@Fe-N-C exhibits remarkable power density, surpassing the Pt/C benchmark. This work offers an effective synthetic strategy for preparing electrocatalysts with excellent ORR performance in zinc-air batteries.
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