JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Fuad Abduro Bushira,Shimeles Addisu Kitte,Haijuan Li,Lirong Zheng,Ping Wang,Yongdong Jin
Simultaneous highly sensitive and accurate detection of dopamine (DA) and uric acid (UA) is of great importance since they are important biomolecules that are commonly coexisted in the human body and play a crucial role in numerous physiological and pathological features. In this work, Fe-N 5 single atom catalyst (SAC) supported on graphene was firstly employed for simultaneous electrochemical detection DA and UA. Owing to its unique electronic structure and abundant active sites, under optimal conditions, the enzyme-like Fe-N 5 SAC constructed electrochemical (bio)sensor exhibits excellent linear characteristic responses in the range of 0.005–500 and 0.01–480 µM, as well as the low limit of detection of 0.007 and 0.027 nM for DA and UA, respectively. More critically, the developed electrochemical system shows promising merits of exceptional stability, good repeatability, and, consequently, it was successfully applied for simultaneous sensitive detection of DA and UA in human serum samples.
研究领域:
生物医学工程
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分析化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xinyu Song,Yang Shi,Zelin Wu,Bingkun Huang,Xinhao Wang,Heng Zhang,Peng Zhou,Wen Liu,Zhicheng Pan,Zhaokun Xiong,Bo Lai
The discriminative activities and mechanisms for activation of O-O bond in peroxy compounds via single-atom catalysts (SACs) especially with a higher coordination number (M-N 5 ) are rarely explored. Herein, the atomic catalyst (Fe-SAC) with Fe-N 5 as the active center was constructed, which could simultaneously and effectively activate peroxymonosulfate (PMS), peroxydisulfate (PDS), and hydrogen peroxide (H 2 O 2 ). Density functional theory (DFT) calculations combined with experiments results demonstrated that the degradation efficiencies of acyclovir were corresponding to the changes of O-O bond length in various peroxy compounds. Meanwhile, the experiments exposed that the three oxidants all produced • OH, but the PMS also contained 1 O 2 and Fe(IV)=O, and PDS contained O 2 •- additively. The scale-up experiment showed Fe-SAC could operate steadily for nearly 7 d. Overall, this work unveils the discriminative mechanisms for activation of O-O band in different Fenton-like systems. Moreover, the Fe-SAC with high coordination numbers has excellent catalytic properties and practical performance.
研究领域:
环境科学
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催化化学
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材料科学
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产品关联
DOI
高影响因子
Environmental Science-Nano
·
2024
·Vol. 11
·期 7
·3092-3103
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IF 5.8
Manoj Kumar Panjwani,Feiyu Gao,Ting He,Pan Gao,Feng Xiao,Shaoxia Yang
M–Nx single-atom catalysts (SACs) with a high coordination number (x > 4) are effective catalysts for eliminating organic pollutants, while the origin of SACs with high activity still remains elusive. In this work, we successfully synthesized an Fe–N5 SAC with axial N coordination, which exhibited exceptional catalytic performance by peroxymonosulfate (PMS) activation for degrading 4-chlorophenol (4-CP) in a wide pH range (4.0–10.0). The rate constant of Fe–N5 (2.99 min−1) was 6.36 times higher than that of Fe–N4, and the turnover frequency (TOF) of Fe–N5 was found to be 4–149 times higher than those of state-of-the-art SACs and nanocatalysts reported in the literature for 4-CP degradation by PMS activation. Moreover, Fe–N5 was not significantly affected by coexisting substances (HA, HCO3−, SO42−, H2PO4−, NO3−, and Cl−) and had satisfactory degradation efficiency for various chlorophenols. Electron paramagnetic resonance (EPR), quenching experiments, and radical probe experiments demonstrated that 1O2 played a key role in the Fe–N5/PMS system for 4-CP degradation. Density functional theory calculations confirmed that a narrower gap between the Fe-3d band center and Fermi level enhanced the electron transfer in Fe–N5, which resulted in promoted PMS activation. In addition, the Fe–N5/PMS system showed good potential for application in real wastewater. The above findings offer important implications for the future of coordination chemistry in designing M–Nx–C SACs (x > 4), highlighting their practical applications in environmental remediation.
研究领域:
环境化学
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催化
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材料科学
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环境工程
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·10455
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IF 15.7
Jin Sijia,Tan Wenxian,Huang Yilin,Wang Yi,He Zhiqiao,Zhang Haiyan,Song Shuang,Cai Yaqi,Zeng Tao
Fe-N 5 single-atom catalysts (SACs) hold great promise for water decontamination, however, the fundamental relationship between their high coordination shell environment and catalytic performance in Fenton-like reactions remains poorly understood. Here, we precisely regulate the high coordination shell defects of a model SAC with well-defined axial Fe-N 5 configurations to elucidate the impact of remote interactions on peroxymonosulfate (PMS) activation. Experimental and theoretical studies confirm that remote modulation of Fe-N 5 sites through high coordination shell defects profoundly enhance Fenton-like catalytic activity, enabling FeN 5 -SD 2 to achieve a turnover frequency (TOF) value of 0.338 min⁻ 1 , surpassing state-of-the-art SACs. Our findings reveal a critical volcano-type correlation between defect content and catalytic efficiency, where coordinated modulation of Fe d -band center positioning and PMS adsorption energetics governs reaction dynamics. Only the FeN 5 -SD 2 configuration with an optimal level of defects density and moderate adsorption energy enables sufficient O-O bond elongation in PMS to lower the energy barrier for selective singlet oxygen ( 1 O 2 ) evolution. This study unveils the mechanistic role of higher coordination shell defects in regulating Fe-N 5 active sites and introduces a well-defined model to investigate the structure–property correlations of higher coordination shells in SACs for Fenton-like reactions.
研究领域:
环境催化
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材料科学
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高级氧化技术
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单原子催化
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可持续水处理
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Tao Gong,Huifang Xu,Xulei Sui,Zhaoyang Han,Ruihui Gan,Longji Yuan,Yuzhe Liu,Huici Qiao,Yongping Zheng,Zhenbo Wang
Rational design integrating curvature and axial coordination enhances both activity and stability. • OTD induced strategy rivets the curved Fe–N 5 sites into porous graphitic carbon. • In MEA tests, the catalyst achieves 1.37 W cm −2 peak power,loses only 10.2% after 10k cycles, and retains 74.3% current at 0.65 over h. • Curved Fe–N 5 motifs tune electronic states and offer triple protection against Fe dissolution, carbon corrosion, and H⁺ attack. Fe–N–C exhibits exceptional catalytic activity and stands as a prominent representative of single-atom catalysts (SACs). However, the activity and, especially, the stability of its active sites pose a formidable challenge for practical applications. Therefore, we first performed DFT predictions on active site structural models featuring curvature and axial coordination, revealing that the curved Fe–N 5 configuration simultaneously boosts both the activity and stability. Then we adopt an O-Tolidine molecular-induced strategy to construct the curved graphitic carbon layers, which anchor Fe single atoms in a bent and axial N-coordinated configuration. The molecular-assisted effect facilitates micropore formation, accelerates the graphitization process, and simultaneously provides additional nitrogen coordination sites, ultimately achieving the curved Fe–N 5 configuration. The curved Fe–N 5 motifs establish a triple protection mechanism: resistance to Fe dissolution, suppression of carbon corrosion and shielding against H⁺ attack, thus alleviating the long-standing activity–stability trade-off in SACs. Benefiting from these structural merits, the as-obtained catalyst delivers outstanding durability in H 2 -O 2 fuel cell, achieving a high peak power density of 1.37 W cm −2 with only 10.2% performance degradation after 10,000 square-wave cycles—far lower than the 29.8% loss of conventional Fe–N–C. Under H 2 -Air conditions at 0.65 V, it retains 74.3% of its initial current density over 200 h. Download: Download high-res image (242KB) Download: Download full-size image
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 14
·4209-4220
·
IF 7
Yujun Wu,Xiaoyang Wang,Bianbian Tian,Wei Shuang,Zhengyu Bai,Lin Yang
Optimizing the adsorption energy of intermediates by precisely modulating the coordination structure of single-atom M–Nx–C electrocatalysts to significantly improve the oxygen reduction reaction (ORR) performance still remains a great challenge. In this work, guided by density functional theory (DFT) calculations, an axial coordination FeN5 single-atom catalyst was constructed by way of an FeN4 species anchored with the N atom from nitrogen-doped graphene to promote the ORR catalytic performance. The special coordination structure of FeN5 can significantly optimize the adsorption of the reaction intermediate and reduce the overpotential of the ORR process compared to that of the FeN4 planar structure, which is commonly used. Hence, the constructed axial coordination FeN5 single-atom catalyst shows extraordinary ORR catalytic performance (Eonset/Ehalf-wave = 0.992/0.916 V vs. reversible hydrogen electrode (RHE), JL = 6.06 mA cm−2 and a 93.9% current retention after 15 h) and a maximum power density of 141 mW cm−2 in a zinc–air battery, which is superior to those of commercial Pt/C. These findings provide new insights into the construction of high-efficiency ORR catalysts from the design of a single atom coordination environment.
研究领域:
材料科学
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电催化
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理论计算
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产品关联
DOI
高影响因子
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