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Nano-Micro Letters · 2024 ·Vol. 17 ·期 1 ·1-16 · IF 31.6

Integration of Electrical Properties and Polarization Loss Modulation on Atomic Fe–N-RGO for Boosting Electromagnetic Wave Absorption

Zhang Kaili,Yan Yuefeng,Wang Zhen,Ma Guansheng,Jia Dechang,Huang Xiaoxiao,Zhou Yu

Single-atom Fe–N 4 sites embedded into graphene were successfully synthesized to exert the dielectric properties of graphene. The absorption mechanisms of metal-nitrogen doping reduced graphene oxide mainly include enhanced dipole polarization, interface polarization, conduction loss and defect-induced polarization. Excellent reflection loss of − 74.05 dB (2.0 mm) and broad effective absorption bandwidth of 7.05 GHz (1.89 mm, with filler loading only 1 wt%) were obtained.

研究领域: 材料科学 · 电磁学
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FOOD CHEMISTRY · 2023 · IF 8.8

A dual-functional single-atom Fe nanozyme-based sensitive colorimetric sensor for tannins quantification in brandy

Xinrou Wang,Huan Liu,Cailin Qiao,Yi Ma,Huibo Luo,Changjun Hou,Danqun Huo

Traditional methods of tannins detection suffer from complex pretreatment, long detection time, and limited sensitivity. Modern techniques like liquid chromatography require expertise, involve tedious result processing, and lack effective data visualization. Therefore, there is a need for an alternative detection method that simplifies pretreatment and detection steps, reduces analysis time, and provides visualized results. In this study, a novel colorimetric sensor based on single-atom Fe nanozyme (Fe@CN-20) was developed for tannins detection. Fe@CN-20 exhibited laccase-like and oxidase-like activities, enabling simultaneous oxidation of tannins and a substrate called TMB. Tannins competed with TMB, allowing quantification of tannins content. The Fe@CN-20/TMB system provided a detection range of 5–100 mg/L tannic acid, with a detection limit of 0.13 mg/L (S/N = 3). Analysis time was approximately 30 min. The platform successfully quantified tannins in brandy, showing less than 5% deviation compared to the standard method. The sensor was simple, sensitive, rapid, and provided strong visualization.

研究领域: 分析化学 · 食品科学 · 纳米技术
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WATER RESEARCH · 2025 · IF 12.4

Single-atom Fe-decorated N-doped porous carbon from waste biomass as a high-performance air-cathode for wastewater treatment in microbial fuel cells

Huanran Liu,Qinyan Yang,Chen Wang,Yang Wu,Li Liu,Guoqing Shen,Qincheng Chen

Microbial fuel cells (MFCs) offer great potential for simultaneous wastewater treatment and energy generation, yet the development of cost-effective and efficient carbon-based cathode alternatives to Pt/C for oxygen reduction reactions remains challenging. This study presents a novel single-atom Fe-decorated N-doped porous carbon (Fe-SA/NBC) synthesized from biogas residue for wastewater treatment. The Fe-SA/NBC demonstrated superior catalytic performance, achieving a kinetic current density of 18.89 mA·cm - ² compared to 10.38 mA·cm - ² for Pt/C, and an enhanced electrochemical surface area with a C dl of 1.81 mF·cm - ² versus 1.76 mF·cm - ² for Pt/C. When integrated into an MFC air-cathode under actual sewage, Fe-SA/NBC outperformed Pt/C, achieving a 22.6 % higher power density (882.92 mW·m - ² vs. 719.81 mW·m - ²), a higher output voltage (0.53 V vs. 0.47 V), and a longer operational duration (3.6 days vs. 3.2 days). Additionally, Fe-SA/NBC exhibited superior removal efficiencies for chemical oxygen demand and ammonia nitrogen during sewage treatment. In practical applications, MFCs equipped with Fe-SA/NBC successfully powered diodes and timers in series-connected configurations. This study introduces an innovative method for producing cost-effective and efficient cathode catalysts from waste biomass, offering significant potential for wastewater treatment and power generation systems.

研究领域: 环境科学 · 材料科学 · 生物学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-10 · IF 16.6

Cell-inspired design of cascade catalysis system by 3D spatially separated active sites

Wang Qiuping,Chen Kui,Jiang Hui,Chen Cai,Xiong Can,Chen Min,Xu Jie,Gao Xiaoping,Xu Suowen,Zhou Huang,Wu Yuen

Cells possess isolated compartments that spatially confine different enzymes, enabling high-efficiency enzymatic cascade reactions. Herein, we report a cell-inspired design of biomimetic cascade catalysis system by immobilizing Fe single atoms and Au nanoparticles on the inner and outer layers of three-dimensional nanocapsules, respectively. The different metal sites catalyze independently and work synergistically to enable engineered and cascade glucose detection. The biomimetic catalysis system demonstrates ~ 9.8- and 2-fold cascade activity enhancement than conventional mixing and coplanar construction systems, respectively. Furthermore, the biomimetic catalysis system is successfully demonstrated for the colorimetric glucose detection with high catalytic activity and selectivity. Also, the proposed gel-based sensor is integrated with smartphone to enable real-time and visual determination of glucose. More importantly, the gel-based sensor exhibits a high correlation with a commercial glucometer in real samples detection. These findings provide a strategy to design an efficient biomimetic catalysis system for applications in bioassays and nanobiomedicines.

研究领域: 生物化学 · 纳米医学 · 仿生学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2021 ·Vol. 23 ·期 8 ·4690-4699 · IF 3.676

An insight into the reaction mechanism of CO2 photoreduction catalyzed by atomically dispersed Fe atoms supported on graphitic carbon nitride

Zhengyan Zhao,Wei Liu,Yantao Shi,Heming Zhang,Xuedan Song,Wenzhe Shang,Ce Hao

We report a combination of experimental and computational mechanistic studies for the photoreduction of CO2 to CO with water, catalyzed by single-atom Fe supported on graphitic carbon nitride (g-C3N4). Density functional theory (DFT) and time-dependent DFT (TDDFT) methods were utilized to explore the behavior of single-atom Fe in g-C3N4, which is of vital importance to the understanding of the CO2 reduction reaction (CO2RR) mechanism. The calculation results reveal that the rate-limiting step of the hydrogen-bonded complex in the absence of Fe atoms is the cleavage of C–O bonds in COOH radicals during the whole CO2RR, which includes the photophysical and photochemical processes. The presence of Fe atoms not only activated CO2 in the ground state and increased the rate constant of the limiting step in the photophysical process, but also functioned as the catalytic active center, lowering the reaction barrier of the C–O bond cleavage in COOH˙ in the photochemical process and resulting in improved photocatalytic activity. In addition, DFT calculations further demonstrated that the electron and proton transfer involved in the photophysical and photochemical processes is closely related to and induced by the hydrogen bonds in the excited state.

研究领域: 材料科学 · 催化化学 · 环境科学
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ACS Nano · 2018 · IF 13.709

High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes

Sufeng An,Guanghui Zhang,Tingwen Wang,Wenna Zhang,Keyan Li,Chunshan Song,Jeffrey T. Miller,Shu Miao,Junhu Wang,Xinwen Guo

Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis. However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation. Herein, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 18.2 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe Mössbauer spectroscopy. The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes. The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions.

研究领域: 材料科学 · 环境化学 · 催化化学
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SOLID STATE SCIENCES · 2025 · IF 3.3

High-dispersed single-atom Fe on N-doped biochar for efficient degradation of organic contaminants by activating peroxymonosulfate

Shutian Lin,Xinli Zhang,Yingzhi Chen,Yuanhong Zhong,Gao Cheng,Lin Yu

The Fe-N-C catalyst was synthesized using loofah sponge-derived carbon and applied for peroxymonosulfate (PMS) activation to degrade organic pollutants. The catalyst, featuring highly dispersed single-atom Fe on the N-C framework, showed outstanding activity for phenol degradation across a wide pH range. The incorporation of Fe significantly boosted the catalytic performance, achieving rapid degradation of phenol at 20 mg L −1 within 10 min, using 0.5 mmol L ‒ 1 of PMS and 0.2 g L −1 of catalyst. Electron paramagnetic resonance (EPR) and reactive oxygen quenching experiments identified the singlet oxygen ( 1 O 2 ) and superoxide radical (O 2 •‒ ) as the main reactive oxygen species, with the former playing a key role. It has been demonstrated that the Fe-N x structures were the active sites that facilitated the generation of 1 O 2 , thereby enhancing the catalytic activity of the Fe-N-C materials. The catalyst also effectively addressed pollutants like Rhodamine B and climbazole, indicating its potential for environmental remediation. The synthesis approach for Fe-N-C is applicable to other transition metals, such as Mn, Co, Ni, Cu, and Zn, providing valuable insights for the development of highly efficient and durable M-N-C catalysts.

研究领域: 环境科学 · 催化材料
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

A hierarchically ordered porous Fe, N, S tri-doped carbon electrocatalyst with densely accessible Fe-Nx active sites and uniform sulfur-doping for efficient oxygen reduction reaction

Hao Han,Xiaomei Wang,Xu Zhang

Doping Fe N C catalysts with heteroatoms has been widely recognized as a most promising way to improve the electrocatalytic activity to achieve the replacement of Pt-based electrocatalysts for efficient oxygen reduction reaction (ORR). However, it is still a challenge to combine delicate control of the catalyst structure with heteroatom-doping to achieve optimal electrocatalytic efficiency. Herein, a strategy of combining chemical vapor deposition (CVD) with dual-template cooperative pyrolysis was rationally designed to synthesize the novel electrocatalyst with densely isolated single Fe atoms scattered on hierarchically ordered porous N and S codoped carbon (ISA-Fe/HOPNSC). The three-dimensional hierarchically ordered interconnected macro/mesoporous structure and uniform sulfur-doping make ISA-Fe/HOPNSC exhibit superb ORR performance in both alkaline and acidic electrolytes with a positive half-wave potential (0.920 V in 0.1 M KOH and 0.795 V in 0.5 M H 2 SO 4 ) as well as outstanding methanol tolerance and long-time stability. As cathode catalyst in Zn-air battery, ISA-Fe/HOPNSC also provides much better maximum power density (210.7 mW cm −2 ) and specific capacity (796.7 mAh g Zn −1 ) than those of Pt/C (112.6 mW cm −2 and 712.6 mAh g Zn −1 ). Remarkably, the synthesis strategy in this work proposes myriad opportunities for combining delicate control of the catalyst structure with heteroatom doping to synthesize high-performance ORR catalysts.

研究领域: 材料科学 · 电化学 · 催化科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Monoatomic Fe-N2O2 sites and carboxyl groups in biochar synergistically driving HV-Fe(IV) dominated peroxymonosulfate activation for anilines degradation

Ting Zhou,Wenyi Dong,Xuechuan Li,Weigang Liu,Mengke Qiang,Hongjie Wang

High-valent ferric oxide species (HV-Fe(IV)) has been increasingly explored to selectively and efficiently remove pollutants from wastewater owing to its high reduction potential, long lifetime, and valuable resistance to anions. However, the directional production of HV-Fe(IV) and its mechanism remain challenging. Herein, a biochar-based catalyst with monoatomic Fe-trans-N 2 O 2 configuration and rich COOH group (SAFe-NKBC) was rationally constructed via KOH and supramolecular organic framework co-pyrolysis. As a result, the SAFe-NKBC/PMS system exhibited exceptional catalytic performance, achieving rapid sulfamethoxazole degradation (97.4% within 10 min) and TOC removal (73.1%). Mechanistic investigations revealed the cooperative catalytic role of single-atom Fe-trans-N 2 O 2 and COOH in biochar support via surface-confinement effect in boosting peroxymonosulfate activation and directional HV-Fe(IV) generation, mediating spatially coupled electron transfer and promoting selective oxidation pathways. Furthermore, a structure–activity relationship for various para-substituted anilines was systematically established via quantitative structure–activity relationship modeling based on different adsorption and oxidation descriptors. The valid descriptors were confirmed to predict reactivity, offering a molecular-level framework for water purification. Meanwhile, the catalyst demonstrated excellent resistance to matrix interference, long-term stability in flow-through systems, and significantly reduced toxicity of degradation byproducts, underscoring its potential in sustainable and precision-oriented water remediation. This work offered new insights into rational SAC design and reactivity prediction for sustainable water remediation.

研究领域: 环境科学 · 催化化学 · 水处理技术 · 材料科学 · 化学工程 · 环境修复
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Single-atom Fe with Fe-N4F1 structure showing superior performances for semi-hydrogenation of alkynol

Haiyang Xie,Dan Tang,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Hongbing Ji,Tao Gan

The design of non-noble metal single-atom catalysts (SACs) with superior performance for semi-hydrogenation of alkynol to alkenol is remarkable but challenging. Herein, fluorine-tuned Fe SACs supported on N, F-codoped carbon (Fe 1 -NFC) with a Fe-N 4 F 1 structure is successfully prepared via a complexation method. The axial F-doping can modulate the electronic structure of the metalloporphyrin-like active sites (Fe-N 4 ), promoting the transfer of electrons from Fe atoms to F atoms to form electron-deficient Fe δ+ species. As a result, the Fe 1 -NFC catalyst shows a remarkable activity for the semi-hydrogenation of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol under mild conditions, with a TOF of 9163 h −1 and a selectivity of 96 % at 97 % conversion, both much higher than that of the Fe SACs supported on N-doped carbon (Fe 1 -NC). Density functional theory (DFT) calculations reveal that the excellent catalytic activity is attributed to the interfacial electronic effect of Fe species induced by axial F-doping, thereby enhancing the exothermic adsorption of alkynol on the Fe-N 4 F 1 structures and accelerating the desorption of alkenol to against the overhydrogenation.

研究领域: 催化 · 材料科学 · 化学工程 · 理论化学
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