JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Meng Cheng,Junhao Liu,Hao Jiang,Chunling Li,Shuangqing Sun,Songqing Hu
In view of the critical importance of oxygen to corrosion evolution, to starve corrosion via depleting oxygen in coatings is a promising strategy. In this work, a novel nanocatalytic anticorrosion concept is proposed to design new coating with outstanding corrosion resistance . Different from the passive barrier of traditional coatings and self-repair after corrosion of current stimuli-feedback coatings, such coating could spontaneously eliminate internal diffused oxygen and greatly suppress the corrosion process. As a proof of concept, single-atom Fe-N-C electrocatalyst with isolated FeN 4 active sites is synthesized by a simple confined carbonization method, exhibiting excellent oxygen reduction performance (E 1/2 = 0.902 V). In composite coating , the evenly dispersed Fe-N-C compensates for the coating defects and serves as oxygen scavengers, which could actively adsorb and consume ambient oxygen, thereby preventing oxygen penetration to the metal substrate surface, eliminating the oxygen contribution to corrosion and significantly boosting the anticorrosion performance of epoxy coating. This in-situ mediation for oxygen in coating prevents metal substrate from receiving new supply of oxygen, while imparting active anticorrosion property to the coating.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Tao Jiang,Weiling Luan,Yufeng Ren,Chenyao Fan,Qi Feng,Lyudmila Turyanska
Exploring an economical and efficient oxygen reduction reaction (ORR) is an essential but challenging field of study. Metal–organic frameworks (MOFs) have emerged as promising candidates for the preparation of porous catalysts. Here we propose a synergistic heat treatment (SHT) method to synthesize Fe–N–C-SHT catalyst with hierarchical porous hollow structures via a simple carbonization method by the synergistic heating of ZIF-8-Fe (ZIF-8 doped with Fe) and ZIF-67 in a tube furnace. Fe–N–C-SHT catalyst displays efficient ORR activity (half-wave potential ( E half ) = 0.88 V versus reversible hydrogen electrode (RHE) with a loading of 0.204 mg Fe-N-C-SHT cm −2 ), which is superior to that of Fe–N–C synthesized using individual heat treatment (IHT) ( E half = 0.84 V) and Pt/C catalyst ( E half = 0.86 V). We achieve enhanced catalytic properties, enhanced methanol tolerance, and long-term durability of the Fe–N–C-SHT catalyst in alkaline electrolyte . The improved ORR activity is attributed to the synergistic effect of Fe doping and optimized SHT methodology, which led to the formation of a highly porous catalyst with numerous active sites. The developed SHT method presents a novel route to fabricate Fe–N–C catalysts with hollow-mesoporous-microporous structures and high performance in ORR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Rui Li,Xiaoxuan Sun,Ling Yang,Panpan Zhao,Jianguo Zhao,Jiao Ding,Shuangli Wu,Chenguang Li,Hao Liu,Shaojun Dong
Curbing the rapid structural degradation of Fe-N-C materials during acidic oxygen reduction reaction (ORR) has been a long-standing challenge in commercializing ORR-based device with long-term stability. Herein, structural deactivation is effectively inhibited via optimizing interfacial Fe-O dipole by introducing the second Fe atom. The elaborately designed Fe double-atom catalysts (Fe DACs), featuring Fe₂N₆ motifs, induce a shift in O 2 adsorption geometry from end-on to bridge configurations for reorienting interfacial Fe-O local dipole ( μ L ) to relieve demetallation. Hence, Fe DACs achieve enhanced operational stability by 10.4 and 31.2 times over Fe 1 N 4 in both single electrode systems and H 2 O 2 -O 2 fuel cells. In-situ measurements and theoretical simulations reveal the origin for the suppression of structural degradation is due to that the optimized Fe-O μ L reduces the tensile stress exerted by the electric field on the Fe-N bond, coupled with intrinsically stable electronic structure in Fe₂N₆ during dynamic structural evolution to stabilize Fe-N bonds.
研究领域:
催化化学
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电化学
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材料科学
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能源化学
·
表面科学
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DIAMOND AND RELATED MATERIALS
·
2026
·
IF 5.2
Yongzhi Zhao,Gengchen Bai,Wenhe Yu,Jianfang Liu,Baorui Jia,Xuanhui Qu,Mingli Qin
The development of efficient non-precious metal catalysts for the oxygen reduction reaction (ORR) is crucial for advancing sustainable energy technologies. Although single-atom Fe–N–C materials hold great promise, they are often limited by metal aggregation issues associated with conventional carbon supports. In this study, we propose a novel catalyst design that stabilizes Fe–N–C single-atom sites on a robust diamond-based matrix to fabricate a highly efficient electrocatalyst. With mild graphitization of the diamond surface to enhance its electrical conductivity during electrocatalytic processes, the Fe species are atomically dispersed and form coordinate covalent bonds with pyridinic N. In alkaline electrolyte, the Fe–N–D catalyst exhibits enhanced ORR activity, outperforming both pristine diamond and carbon black reference samples. Density functional theory (DFT) calculations reveal that the active Fe–N 4 –C configuration promotes kinetically efficient ORR by optimizing charge transfer and weakening the O O bond. This work integrates conductive sp 2 ‑carbon with a stable sp 3 -diamond core to establish a novel support for anchoring single-atom catalysts, providing a new substrate materials-design paradigm for electrocatalysis. Download: Download high-res image (124KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Wenhao Zhang,Chuanyi Zhou,Jiahao Cui,Canglou Liu,Yongfang Rao,Wei Yan
Current adsorbents for bisphenol A (BPA) require complex preparation and relatively low adsorption capacities. Here, a high-performance adsorbent (Fe-N-C) was synthesized from iron-modified zeolite imidazole frameworks-8 (ZIF-8) via pyrolysis. With an exceptionally high specific surface area of 1565.15 m 2 ·g −1 , Fe-N-C removed 90% of BPA within 10 min and achieved adsorption equilibrium within 3 h. Furthermore, Fe-N-C exhibited a maximum BPA theoretical adsorption capacity of 877.45 mg·g −1 (288 K). The adsorption kinetics and isotherms conform to pseudo-second-order kinetics and the Langmuir model. Fe-N-C also demonstrated excellent performance across a wide pH range (4–10) and in complex water matrix. The high adsorption capacity was primarily attributed to π-π interactions, along with hydrogen bonding, electrostatic interactions, and hydrophobic interactions. Notably, in addition to efficiently adsorbing BPA, Fe-N-C exhibited a high selectivity toward organic compounds with two benzene rings by π-π interactions, such as bisphenol B (BPB), 2,2-bis (4-aminophenyl) propane (BAPP) and diclofenac (DCF) due to the mediation of graphitized microdomains. This study provides a simple route to prepare high-capacity N-doped carbon adsorbents for the selective and rapid adsorption of specific structural pollutants.
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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.
研究领域:
材料科学
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电化学
·
传感器技术
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·062501
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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.
研究领域:
材料科学
·
电化学
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ANALYTICA CHIMICA ACTA
·
2023
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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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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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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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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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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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