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Energy Storage Materials · 2024 · IF 18.9

Using CrN4 moiety to weaken the dissociation barrier of hydroxyl on adjacent single iron atom for efficient oxygen reduction

Lilian Wang,Li Yang,Xinyu Zhao,Hang Ma,Bohuai Pang,Lingyan Duan,Kun Zeng,Lu Liu,Anran Chen,Hong Guo

The strong perturbation of the valence band within the entire material system and accelerated *OH dissociation from Fe site are triggered by incorporating CrN 4 moiety with low Fenton effect and *OH adsorption energy. This atomically dispersed Cr=N 2 =Fe electrocatalyst is developed by adopting a super time-/energy-saving Joule heating strategy (∼ 10 s). Through the investigation of valence orbital energy levels and valence electron behavior for the prepared catalysts, in combination with in-situ Raman testing and theoretical calculations, we have determined that the interaction between the metal sites and oxygen-containing intermediates primarily depends on orbital energy levels before being further evaluated by bond order involving electronic modulation. This finding may offer a valuable insight for future research in related electrocatalysis fields. The Cr=N 2 =Fe catalyst exhibits higher ORR catalytic capability than commercial Pt/C, thus driving stable operation of the assembled zinc-air battery for over 300 h.

CAS / MDL: 7440-06-4 12036-10-1
研究领域: 材料科学 · 电催化 · 能源化学
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Materials Today Bio · 2025 · IF 10.2

Enhancing the Antioxidant Capacity of Fe Single-Atom Nanozymes through Local Coordination Manipulation for Psoriasis Treatment

Hongjin Xue,Yunqian Li,Xinyu Ma,Qi Zhang,Junkai Zhu,Xiaoli Ni,Jianfeng Qiu,Zhengjun Li,Zhen Mu

Psoriasis is a chronic skin condition with significant unmet medical needs, characterized by high levels of reactive oxygen species (ROS) and accompanying oxidative stress. In this study, we developed a novel single-atom iron nanozyme (Fe-N 3 ), designed to mimic natural antioxidant enzymes, for the effective treatment of psoriasis. By optimizing the local coordination environment of Fe atoms, Fe-N 3 demonstrated superior superoxide dismutase (SOD), catalase (CAT), ascorbate peroxidase (APx), and glutathione peroxidase (GPx)-like activities compared to Fe-N 4 . These properties enable efficient ROS scavenging and oxidative stress alleviation. Theoretical analyses revealed that Fe-N 3 possesses lower energy barriers for ROS decomposition, explaining its superior catalytic performance. Furthermore, in vitro and in vivo experiments have demonstrated that Fe-N 3 nanozyme exhibited remarkable therapeutic effects with extremely low cytotoxicity, effectively inhibiting pathological epidermal proliferation, downregulating key inflammatory factors, and reducing the expression levels of psoriasis-associated pathway proteins. This work highlights the promise of single-atom nanozymes in the curing of inflammatory skin diseases, advancing the transformative role of nanotechnology in biomedicine.

研究领域: 生物医学 · 纳米技术 · 皮肤病学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Aunano-Fe1 tandem catalysis for promoted methane conversion to acetic acid by O2 oxidation

Zhen Wang,Lei Ying,Weibin Xu,Beien Zhu,Chuande Huang,Pengfei Wu,Qingqing Gu,Bing Yang,Jian Lin,Yi Gao,Xiaodong Wang,Tao Zhang

Tuning metal size from nanoscale to uniform single atoms holds the potential to promote the oxygenates selectivity for direct methane conversion, but suffers from low kinetics when utilizing O 2 as oxidant. Herein, we report a Au nano -Fe 1 -ZSM-5 catalyst for enhanced acetic acid production from CH 4 , CO, and O 2 in aqueous solution. The Au nano nanoparticles enable upgrading of O 2 into active hydroxyl radicals (•OH) via net reaction between O 2 , H 2 O and CO. The Fe 1 single atoms within 5-nm range from Au nano could be converted into active Fe 1 IV -O by •OH oxidation, which catalyzes rapid H-abstraction from CH 4 and subsequent C-C coupling with CO for acetic acid production. Such closely adjacent but separate active centers, i.e., Au nano and Fe 1 for decoupled O 2 and CH 4 activation, respectively, enable a high reactivity of 982 mmol/g metal /h for methane conversion with O 2 oxidant while retaining a high acetic acid selectivity of 81 % at 150 °C.

研究领域: 催化化学 · 能源化学 · 环境科学
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Materials Today Communications · 2025 · IF 4.5

Highly efficient adsorption and degradation of zearalenone by Fe single-atom N-doped porous carbon: Degradation mechanisms and pathways

Zhilei Zhao,Yu Li,Wenlei Zhai,Liuqing Wang,Qianqian Li,Yudan Wang,Meng Wang

The contamination of highly toxic zearalenone (ZEN) in food and the environment poses a serious threat to human safety. However, it is still challenging to establish an efficient, inexpensive and stable ZEN degradation technology. In this study, a Fe single-atom nitrogen-doped porous carbon (Fe-N-PC) was synthesized by high-temperature pyrolysis and used for efficient adsorption and degradation of ZEN. Fe-N-PC showed a high adsorption capacity (q m = 78.2 mg/g) for ZEN, and the Fe-N-PC/peroxymonosulfate (PMS) system could remove 99.39 % of ZEN, in which 1 O 2 played a major role in ZEN degradation. Furthermore, four degradation products of ZEN were identified and possible degradation pathways were hypothesized. For practical applications, Fe-N-PC was applied to remove ZEN from Coix seed extracts, and the results showed that Fe-N-PC was able to detoxify ZEN from Coix seed (92.32 %). Additionally, Fe-N-PC and ZEN degradation products showed low biological toxicity. In a word, the Fe-N-PC/PMS system was used for efficient adsorption and degradation of ZEN, and has been practically applied in complex food matrices, demonstrating Fe-N-PC may be a promising material for the removal of ZEN in the food field.

CAS / MDL: 7664-39-3
研究领域: 食品安全 · 环境科学 · 材料科学
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iScience · 2023 · IF 5.8

Iron atomic cluster supported on Co/NC having superior water oxidation activity over iron single atom

Jian Du,Yunxuan Ding,Yu Guo,Licheng Sun,Fei Li

Carbon-supported iron-cobalt bimetallic electrocatalysts usually exhibit robust catalytic activity toward the oxygen evolution reaction (OER). However, the spatial isolation of Fe species at atomic level on cobalt-carbon solid remains a great challenge for practical catalytic applications in the OER. Here, we report the fabrication of CoFe bimetal porous carbon electrocatalysts by pyrolysis of molecularly defined iron complexes such as FePc (Pc = phthalocyanine) and Fe(acac) 3 pre-encapsulated in the cavities of zeolitic imidazolate framework (ZIF)-67. With this unique strategy, high-loading atomic Fe nanoclusters (Fe-ACs) and Fe single atoms (Fe-SAs) were supported on Co/NC hybrids relying on the size of the molecular Fe precursors. The former exhibited superior OER performance to the single Fe atom-decorated Co/NC, as well as other ZIF-67-derived electrocatalysts. Theoretical modulation suggests Co as the OER active site for Fe-ACs@Co/NC at the in situ -formed FeOOH-ACs/Co 3 O 4 interface, while Fe was proposed as the active site for Fe-SAs@Co/NC.

研究领域: 材料科学 · 电化学
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Single-atom iron fabricated electrochemical flexible sensor for detection of hypochlorite ions in water samples

Xin Chen,Zhujun Zou,Zhengyi Cang,Min Wang,Juejin Teng,Hong Bin Yang,Chunxian Guo,Fangxin Hu

Precisely measuring hypochlorous ions (ClO − ) concentration in water is crucial for ensuring safe disinfection, maintaining water quality, and protecting public health. A single-atom iron (Fe/GO) based flexible electrochemical sensor was developed for high sensitive monitoring of ClO − . The electrode kinetic processes were investigated in detail. Moveover, results showed that the sensor exhibited a wide linear range toward ClO − from 5.16 × 10 −5 to 0.0253 µM, with good repeatability and stability. The detection of ClO − concentration in various water samples were achieved by the proposed sensor.

研究领域: 环境科学 · 分析化学
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Journal of Energy Chemistry · 2021 · IF 9.676

Boron modulating electronic structure of FeN4C to initiate high-efficiency oxygen reduction reaction and high-performance zinc-air battery

Xue Zhao,Xue Li,Zenghui Bi,Yuwen Wang,Haibo Zhang,Xiaohai Zhou,Quan Wang,Yingtang Zhou,Huaisheng Wang,Guangzhi Hu

The biggest challenge is to develop a low cost and readily available catalyst to replace expensive commercial Pt/C for efficient electrochemical oxygen reduction reaction (ORR). In this research, closo -[B 12 H 12 ] 2− and 1,10-phenanthroline-iron complexes were introduced into the porous metal-organic framework by impregnation method, and further annealing treatment achieved the successful anchoring of single-atom-Fe in B-doped CN Matrix (FeN4CB). The ORR activity of FeN4CB is comparable to the widely used commercial 20 wt% Pt/C. Where the half-wave potential ( E 1/2 ) in alkaline medium up to 0.84 V, and even in the face of challenging ORR in acidic medium, the E 1/2 of ORR driven by FeN4CB is still as high as 0.81 V. When FeN4CB was used as air cathode, the open circuit voltage of Zn-air battery reaches 1.435 V, and the power density and specific capacity are as high as 177 mW cm −2 and 800 mAh g Zn −1 (theoretical value: 820 mAh g Zn −1 ), respectively. The dazzling point of FeN4CB also appears in the high ORR stability, whether in alkaline or acidic media, E 1/2 and limiting current density are still close to the initial value after 5000 times cycles. After continuously running the charge-discharge test for 220 h, the charge voltage and discharge voltage of the rechargeable zinc-air battery with FeN4CB as the air cathode maintained the initial state. Density functional theory calculations reveals that introducing B atom to Fe–N4–C can adjust the electronic structure to easily break O = O bond and significantly reduce the energy barrier of the rate-determining step resulting in an improved ORR activity.

研究领域: 材料科学 · 电化学 · 催化科学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-14 · IF 15.7

Unsaturation degree of Fe single atom site manipulates polysulfide behavior in sodium-sulfur batteries

Song Wanqing,Wen Zhenzhuang,Wang Xin,Qian Kunyan,Zhang Tao,Wang Haozhi,Ding Jia,Hu Wenbin

Sodium | |sulfur batteries hold great promise for grid-scale energy storage, yet their performance is hindered by the shuttling and sluggish redox of sulfur species. Herein, we report a strategic design of sulfur hosts modified with coordinatively unsaturated iron single-atom (Fe‒N x ) for sodium | |sulfur batteries. Utilizing theoretical calculations, geometric descriptor γ ( l Na‒S / l Fe‒N ) and electronic descriptor φ ( e g  / t 2g ) simultaneously correlated with the unsaturation degree of Fe‒N x site are proposed. A negative correlation between γ and the adsorption strength of sodium polysulfides, along with a positive correlation between φ and the decomposition capability of Na 2 S are established. The Fe‒N 1 sites, with the minimum γ and maximum φ values, are identified as the optimal functional species for optimizing polysulfides behaviors. Sodium | |sulfur batteries utilizing Fe‒N 1  /S positive electrodes deliver improved sulfur utilization (81.4% at 167.5 mA g ‒1 ), sustained rate performance (1003.0 mAh g ‒1 at 1675 mA g ‒1 ), and stable cycling (83.5% retention over 450 cycles at 3350 mA g ‒1 ). Moreover, Fe‒N 1 /S positive electrodes enable sodium | |sulfur pouch cells to deliver a sulfur utilization of 77.4% (1296.9 mAh g ‒1 ) at 0.1 A g ‒1 . Our work offers a strategy for designing high-activity, fast redox sulfur positive electrodes and validates the practical potential of sodium | |sulfur batteries.

研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Atomically dispersed iron & iron clusters synergistically accelerate electrocatalytic ammonia synthesis

Haoran Zhang,Yuelong Liu,Sanshuang Gao,Haijian Wang,Rui Bai,Yan Zhao,Yingtang Zhou,Guangzhi Hu,Xue Zhao

Green energy-driven electrochemical-nitrate-reduction-reaction (eNitRR) provides an alternative pathway for sustainable ammonia synthesis, but there is still a lack of reliable catalyst. Herein, through the combination of coordination confinement and spatial confinement, single-atom Fe and Fe clusters were simultaneously embedded on nitrogen-doped-hollow-carbon-tubes (Fe/NHCTs) to cooperatively promote the highly selective conversion of nitrate to ammonia in complex water environments. The ammonia yield rate reached 45595.63 μg h −1 mg −1 with Faradaic efficiency close to 100 %. The Zn-nitrate battery with Fe/NHCTs as the core has a high open circuit voltage and power density, and can output electric energy for a long time while highly selective synthesis of ammonia. The pathway and hydrogenation mechanism of nitrate evolution to ammonia were revealed using the in-situ attenuated total reflection Fourier-transform infrared, online differential-electrochemical-mass-spectrometry and density functional theory calculations, the intermodulation of electrons between single-atom Fe and Fe clusters synergistically accelerates the conversion of nitrate to ammonia.

研究领域: 材料科学 · 电催化 · 能源化学
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Chem Catalysis · 2024 · IF 11.5

Precisely constructing pentagon trapped single-atomic iron sites in defective carbon for efficient oxygen electroreduction

Xin Wang,Hai Sun,Tianwei He,Panjie Guo,Run Huang,Zhelin Mao,Chao Han,Xuan Liu,Mengting Huang,Lei Wang

Precisely controlling the local coordination structure of atomic Fe sites has been widely recognized as the key to attain highly efficient oxygen reduction reaction (ORR) catalysts for replacing Pt-based materials. Here, we use pre-synthesized pentagon-rich defective carbon (PDC) as a matrix material to realize a custom-made pentagon defect-coordinated Fe-C 5 configuration via a chemical vapor deposition method. The intrinsic activity of as-prepared PDC-supported Fe single-atom catalysts (Fe sac -PDC), in terms of specific kinetic current density (J k-specific ), mass activity, and turnover frequency (TOF), is valued to be several times higher than that of other N-coordinated counterparts. Density functional theory (DFT) calculations demonstrate that the excellent ORR activity of pentagon-type Fe-C 5 sites originates from the optimized electronic state with more charge transfer and down-shifted d-band center. Our work gives new insight into boosting the ORR performance of atomic single-site catalysts via purposely and precisely constructing more unique defect-stabilized single atomic species.

研究领域: 材料科学 · 电化学 · 理论计算
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Strengthening the oxygen reduction stability and activity of single iron active sites via a simultaneously electronic regulation and structure design strategy

Yunfeng Zhan,Tianyou Zhao,XiaoXian Wu,Xiaoming Gao,Ruishen Huang,Zehong Zhang,Pingzhen Li,Xiongcong Guan,Chengjie Chen,Xiaojun Liu,Xiufeng Tang,Nan Wang,Hui Meng

Single-atom iron-nitrogen-carbon materials have demonstrated remarkable potential in catalyzing the oxygen reduction reaction (ORR). In this study, a novel approach is proposed for regulating the microenvironment of single iron sites through the coupling of neighboring Zn with an open-mesoporous carbon plane. This structural arrangement effectively modulates the density of states and d-band center of Fe atoms, resulting in moderate adsorption and desorption of oxygen intermediates and thereby reducing the energy barrier of the ORR. Moreover, the open-mesoporous structure ensures the accessibility of the active sites and facilitates the mass transfer of reactants, intermediates, and products during the ORR. Consequently, the synthesized M-Fe-ZnNC catalyst exhibits enhanced ORR performance and excellent stability. This study serves to inspire the exploration of high-performance non-precious metal catalysts for the ORR, leveraging simultaneous electronic regulation and structure design.

研究领域: 材料科学 · 电化学
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Phthalocyanine pyrolysis derived Fe single-atom sites on g-C₃N₄ for enhanced photocatalytic organic pollutant degradation

Tiefeng Xu,Chenyu Li,Ke Xiang,Yingxin Lu,Wangyang Lu

The photocatalytic removal of organic pollutants from wastewater has gained significant attention in recent years due to its environmental benefits and cost-effectiveness. In this study, a pyrolytic iron phthalocyanine/graphitic carbon nitride (FePc/g-C 3 N 4 ) composite photocatalyst was synthesized using ball milling and thermal cracking, and its performance in photocatalytic degradation along with the underlying mechanisms was investigated. Under solar light irradiation, the pyrolytic FePc/g-C 3 N 4 photocatalyst achieved complete carbamazepine (CBZ) degradation within 12 min by activating peroxymonosulfate (PMS), demonstrating a 29 % enhancement in degradation efficiency compared to the unpyrolytic FePc/g-C 3 N 4 . Additionally, the stability of the catalyst improved significantly post-pyrolysis, maintaining over 98 % degradation efficiency across nine cycles. The thermal treatment disrupted the phthalocyanine structure, modifying the coordination environment of the central Fe atom and facilitating the transfer of photogenerated charge carriers. This research provides valuable insights for designing stable single-atom iron-based composite photocatalysts.

研究领域: 环境科学 · 材料科学
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