LANGMUIR
·
2025
·
IF 3.9
Yingjin Ma,Qifeng Li,Xueqing Qiu,Zhixian Li
Single-atom nanozymes can accurately mimic the catalytic centers of enzymes at the atomic scale, showing high catalytic efficiency and selectivity. Inspired by the active center of natural laccase, we constructed a nitrogen-doped carbon-based single-atom nanozyme (Fe-NC) featuring planar Fe–N4 active sites using a zeolitic imidazolate framework (Fe/ZIF-8) as a precursor. The resulting Fe–NC showed high laccase-like activity toward phenolic substrates such as 2,4-dichlorophenol, with a catalytic efficiency 77 times higher than that of natural laccase. Furthermore, Fe–NC efficiently catalyzed the degradation of tetracycline hydrochloride (77.14%) under mild conditions, with an activity 13 times that of laccase. It also selectively and oxidatively depolymerized birch lignin into valuable aromatic monomers, including vanillin and vanillic acid. These findings highlight the key role of planar Fe–N4 coordination in improving bioinspired catalysis and reveal the great potential of single-atom nanozymes in biomass valorization.
研究领域:
纳米酶催化
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环境修复
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生物质转化
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材料化学
·
仿生催化
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Lingzhe Meng,Shuwen Niu,Zhengyu Wei,Xue Qin,Faheem Naseem,Wei Wei
Iron phthalocyanine (FePc) with tetracoordinated Fe-N 4 site shows promising activity for catalyzing the oxygen reduction reaction (ORR) in alkaline media. However, the consecutive proton-coupled electron transfer (PCET) steps with water as the proton donor and low electronic conductivity of FePc raise the kinetic barriers for device application. Herein, a significant effect of polyoxometalates (POMs) on the ORR kinetics of Fe-N 4 sites via surface coordination of FePc is revealed. POM clusters modulate the interactive steric/electronic environment of Fe-N 4 , leading to a low barrier for H 2 O cleavage to produce protons along with a high electron transfer rate, thereby accelerating the PCET steps of FePc. With precisely controlled electron charge of POM clusters, the influence and mechanism of heteropoly blue in promoting PCET steps of FePc relative to heteropoly acid are elucidated, and noticeably enhanced ORR activity and reaction current are achieved. These findings highlight the potential of POMs as ligands to optimize dynamics of Fe-N 4 atomic sites toward efficient alkaline ORR.
研究领域:
化学
·
材料科学
·
催化
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jingshun Shen,Qi Liu,Qiqi Sun,Jianwei Ren,Xue Liu,Zuoxu Xiao,Chuanwang Xing,Yuexing Zhang,Guangwu Yang,Yanli Chen
A novel two-dimensional (2D) single-atom Fe/N/C catalyst (Fe 1 Zn 30 NC PDI ) has been prepared upon pyrolyzing a well-designed quasi-Fe-/Zn-phthalocyanine-based polymer (qFePc 1 @qZnPc 30 @PDI). In the qFePc 1 @qZnPc 30 @PDI precursor, qFePc moieties containing Fe-N 4 sites are efficiently segregated by lots of qZnPc moieties connected together by perylene linkers, which not only leads to the larger specific area in the resulting Fe 1 Zn 30 NC PDI but more importantly ensures the in-situ formation of Fe-N 4 sites on the self-supporting 2D N-doped carbon backbone. Impressively, Fe 1 Zn 30 NC PDI exhibites its superior oxygen reduction reaction (ORR) electro-catalytic activity and peroxidase (POD)-like activity. For ORR in an alkaline medium, it exhibites a much higher onset potential of 0.97 V and half-wave potential of 0.89 V than 20 wt% Pt/C catalyst with good durability of 92 % retention rate after 20000 s. And, Fe 1 Zn 30 NC PDI also shows better peak power density (86 mW cm −2 ) compared with 20 wt% Pt/C in Zn-air battery. Benefiting from the specific POD-like activity of Fe-N 4 , the Fe 1 Zn 30 NC PDI also shows excellent and selective performance in colorimetric H 2 O 2 sensing, with the ultrafast response (30 s), a low limit of detection (10 nM), and good robustness. This work sheds light on a promising design concept for synthesizing 2D polymer-derived single-atom multifunctional catalysts.
研究领域:
材料科学
·
电化学
·
分析化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mengxia Shen,Jiale Qi,Kun Gao,Chao Duan,Jun Liu,Qingqing Liu,Hao Yang,Yonghao Ni
Fe-N x C single-atom catalysts have been immensely explored as the most promising ORR catalysts for replacing noble metals. Nevertheless, how to precisely introduce Fe atoms to optimize their spatial distribution and coordination environment in carbonaceous matrices while constructing the hierarchical porous structures to facilitate the mass transport process and ensure the accessibility of Fe-N x sites remain significant challenges. Here, we propose a strategy to prepare porous N -doped carbon aerogels anchored with single atomic Fe sites (Fe-SA@PNC) as highly efficient ORR electrocatalysts via directional freeze-casting and chemical vapor deposition. Fe-SA@PNC exhibit remarkable ORR activity and stability due to the highly stable honeycomb morphology and hierarchical pore structure, as well as the atomically dispersed Fe-N 4 sites in the carbon support. Furthermore, the practical application of Fe-SA@PNC catalysts as cathode materials in Zn-air batteries was demonstrated with encouraging performance. This study provides a promising approach for constructing high-efficiency ORR single-atom catalysts.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Fantao Kong,Yifan Huang,Meixin Chen,Ge Meng,Han Tian,Yafeng Chen,Ziwei Chang,Chang Chen,Wenping Sun,Xiangzhi Cui,Jianlin Shi
The performance of oxygen reduction reaction (ORR) on Fe-N-C single-atom catalysts (SACs) is still less satisfactory due to the rather low atom-utilization of active sites. Here, a novel acetate thermolysis-assisted route is proposed to create hierarchical carbon nanocages of Fe-N-C SACs (Fe SA -N/Cs-OAc) by selective cleavage of carbon layers, which features abundant edge-sited Fe-N 4 moieties in well-defined mesoporous channels. Benefiting from the ultra-high site density and utilization of Fe-N 4 moieties, the optimized Fe SA -N/Cs-OAc catalyst demonstrates excellent ORR activities marked by extraordinarily high half-wave potentials ( E 1/2 ) of 0.94 V and 0.82 V in alkaline and acidic electrolytes. Zn-air battery using Fe SA -N/Cs-OAc as cathode delivers a power density of 165 mW cm −2 , and the maximum output power in H 2 -O 2 fuel cell reaches 640 mW cm −2 . The abundant mesoporosity makes most Fe-N 4 sites accessible and simultaneously produces in-plane pore defects that reduced adsorption energy of *OH (−0.72 eV), finally presenting remarkably enhanced ORR performance.
研究领域:
材料科学
·
电化学
·
催化科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Chao Chen,Shilong Zhou,Jiawei Xia,Le Li,Xingyue Qian,Fengxiang Yin,Guangyu He,Haiqun Chen
Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N 4 sites anchored on N -doped hierarchically porous carbon (Fe-NC-C 3 N 4 ). The optimized Fe-NC-C 3 N 4 exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential ( E 1/2 ) of 0.90 V vs. RHE and a promising low overpotential of 0.305 V vs . RHE at 10 mA·cm −2 in alkaline electrolyte. These superior catalytic activities are attributed to the combined effect between the atomic active sites and the well-balanced micro-meso-macropore structures. The homemade liquid Zn-air battery (ZAB) assembled with Fe-NC-C 3 N 4 catalyst displays a power density of 133.59 mW·cm −2 and a significant energy density of 882.58 mAh·g −1 , exceeding those of the equipment with commercial Pt/C-RuO 2 (56.82 mW·cm −2 and 643.87 mAh·g −1 , respectively). Particularly, the corresponding flexible wearable ZAB manifests outstanding foldability and cyclical stability. This work opens a new perspective for the structural design of single-atom catalysts in the energy storage and conversion area.
研究领域:
材料科学
·
能源存储与转换
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Shichao Cai,Yurou Tan,Hongyi Li,Liwei Yang,Bo Chen,Feng He
Zero-valent iron (ZVI, Fe0) can effectively reduce a variety of chlorinated hydrocarbons. However, ZVI is incapable of dechlorinating 1,2-dichloroethane (1,2-DCA), a commonly found contaminant in groundwater, and the existing ZVI modification methods have little effect on this predicament. In this study, we prepared ZVI composites modified with Fe–N4 coordination structure (Fe0@FeNC), which exhibited outstanding dechlorination performance toward 1,2-DCA. Fe0@FeNC (1 g/L) can degrade 94% of 1,2-DCA (10 mg/L) within 37 days, with an ethene selectivity of nearly 100%, whereas nanoscale ZVI (nZVI) or even Pd-doped nZVI and sulfidated ZVI cannot degrade 1,2-DCA. The results from X-ray diffraction patterns and Mössbauer spectra confirmed the presence of Fe0 and Fe–N4 coordination structure in the Fe0@FeNC, which were proven to be the electron donor and dechlorination active center for 1,2-DCA dechlorination, respectively. Theoretical calculation reveals that the Fe–N4 coordination structure can reduce the free energy required for 1,2-DCA reduction, thus allowing 1,2-DCA to utilize electrons provided by Fe0 to achieve dechlorination. These findings can guide the design of ZVI-based materials to achieve in situ abiotic remediation of 1,2-DCA-contaminated groundwater.
研究领域:
环境科学
·
材料化学
·
化学工程
·
污染修复
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DOI
PubMed
高影响因子
ACS Sensors
·
2026
·
IF 10.9
Fan Shi,Shu Deng,Lianjin Jiang,Jidie Tao,Yongfa He,Jinju Zuo,Brij Mohan,Wei Sun,Qiantao Ma
Chlorogenic acid (CGA) has antibacterial, antiviral, and antioxidant properties, making its detection essential in food science, pharma, and environmental monitoring. Nevertheless, the mechanistic understanding of CGA recognition and redox behavior at electrochemical sensor interfaces remains limited, posing a key scientific challenge. Herein, a novel Fe-N4 diatomic-site carbon nanomaterial is prepared via in situ pyrolysis of coffee grounds, which served as a simultaneous precursor for carbon, iron, and nitrogen. Aberration-corrected scanning transmission electron microscopy confirms single-atom dispersed iron with diatomic active sites. At the same time, X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal a Fe–N4 coordination. Density functional theory calculations indicate that during CGA oxidation, hydroxyl oxygen atoms preferentially adopt a side-adsorption configuration at dual active sites, thereby enhancing interfacial electron transfer and catalytic selectivity. The constructed electrochemical sensor exhibits two linear response ranges, 0.2−0.8 and 0.8−500.0 μmol/L, with a detection limit of 0.067 μmol/L (LOD = 3 s/m). Overall, this study presents a sensitive, cost-effective electrochemical sensor for CGA detection and highlights the critical role of adsorption configuration in determining the performance of single-atom catalysts.
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DOI
PubMed
高影响因子
Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·96
·
IF 36.3
Fang Wenhan,Xu Kailong,Wang Xinlei,Zhu Yuanhang,Li Xiuting,Liu Hui,Li Danlei,Wu Jun
A universal synthetic strategy was proposed to construct heteroatom axially coordinated Fe–N 4 single-atom seawater catalyst materials (Cl–Fe–N 4 and S–Fe–N 4 ).
The Cl–Fe–N 4 catalyst achieves a limiting current density of 5.8 mA cm −2 and a half-wave potential of 0.931 V vs. RHE in alkaline synthetic seawater, outperforming commercial Pt/C (40 wt%).
The seawater-based zinc-air battery fabricated with Cl–Fe–N 4 demonstrates a power density of 187.7 mW cm −2 at 245.1 mA cm −2 and maintains stable cycling performance for 200 h.
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PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Yulong Zhou,Rui Li,Yu Zhou,Chuanping Li,Fengcui Shen,Rongmei Liu,Xiandong Zhu
The design of high-efficient, low-cost, and stable electrocatalysts for oxygen evolution reaction (OER) is highly demanding for energy conversion applications. Metal-organic frameworks (MOFs), with large surface area and flexible molecular species, can supply atom-dispersed metal active coordination sites (M−N X , M−S X , M−O X ) for OER and have been regarded as potential catalysts for practical applications. However, it is still challenging to use MOFs as OER catalysts directly due to their low conductivity and poor stability. Herein, we successfully synthesized a 2D c-MOF of Fe 3 (HITP) 2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) on the surface of nickel foam (NF) by using a layer-by-layer self-assembly strategy. The Fe 3 (HITP) 2 /NF-x electrode (x = 5, 10, 15, 20 is the number of cycles) exhibited impressive OER catalytic activity in alkaline electrolyte (1 M KOH), which is superior or comparable to most of the transition metal-based materials reported. Typically, Fe 3 (HITP) 2 /NF-15 were able to fully expose the Fe-N 4 catalytic sites with an overpotential of 224 mV at a current density of 10 mA·cm −2 and a Tafel slope of 45.4 mV·dec -1 . This was mainly attributed to the higher ECSA value, better kinetic process, and fast charge transfer ability of Fe 3 (HITP) 2 /NF. In addition, the current density of Fe 3 (HITP) 2 /NF-15 remained at 97.3 % of the initial current density after 24 h i-t stability test, showing excellent catalytic stability. This work provided a novel design strategy for the direct application of MOFs to OER applications.
研究领域:
材料科学
·
能源化学
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产品关联
DOI
高影响因子
TALANTA
·
2026
·
IF 6.7
Xiao Ma,Junjie Wang,Xin Chen,Jingcheng Li,Jiaqi Xue,Yufan Hou,Shihao Zhao,Jingxiang Zhao,Xiaomi Meng,Huajun Chen,Fang Wang,Fangya Guo,Jian Sun,Dan Zhao
Oxidase-like nanozymes use dissolved O 2 as the terminal electron acceptor and do not require exogenous H 2 O 2 , offering methodological advantages; however, conventional “one-pot carbonization” often causes concurrent carbonization and active-site formation, making the coordination environment difficult to control. Here, a sequential “pre-coordinate-polymerize-pyrolyze” site-engineering route was developed. On carbon black, OPD-Fe 3+ pre-coordination and in situ oxidative polymerization were carried out, followed by thermal treatment and purification, by which Fe–N moieties were immobilized within the shell region of the material to afford highly dispersed Fe–N x moieties predominantly featuring Fe–N 4 -like coordination (Fe–N 4 @CB d ). Multiscale characterization (XRD/XPS/XANES/EXAFS) consistently showed that iron resided predominantly in a first coordination sphere dominated by Fe–N (coordination number CN ≈ 3.7; R ≈ 2.01 Å), with no resolvable Fe–Fe scattering and only minor, non-dominant Fe-containing phases. ROS-trapping and time-dependent EPR measurements further confirmed continuous O 2 activation with the generation of O 2 • - , •OH, and 1 O 2 in the Fe–N 4 @CB d /O 2 system. DFT calculations additionally supported Fe–N 4 -like Fe–N x sites as the most plausible dominant active structures for O 2 activation. Under a unified TMB/O 2 system, steady-state enzyme kinetics exhibited outstanding performance, with V max = 351 nmol L −1 s −1 and K m = 0.56 mM, which are competitive among reports using the same substrate/readout. An H 2 O 2 -free colorimetric platform for alkaline phosphatase (ALP) was constructed on this material, achieving a low limit of detection and good linearity; acceptable accuracy and precision were verified by standard additions in diluted serum. This sequential strategy predefines the Fe–N neighborhood and topology at the precursor stage, reduces uncertainty in site formation, and avoids metal-organic framework (MOF)/hard-template/ionic-liquid multi-step procedures, thereby providing a strong basis for reproducible Fe–N 4 -like/Fe–N x oxidase-like nanozyme preparation and streamlined, robust bioanalysis.
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高影响因子
INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Huanran Zheng,Yuchao Wang,Jing Zhang,Yu Bai,Yingbi Chen,Peiyao Yang,Md Raziun Bin Mamtaz,Danni Deng,Zechao Zhuang,Houzheng Ou,Meng Wang,Guozhao Fang,Haozhi Wang,Xiang Xiong,Dingsheng Wang,Chuan Zhao,Yongpeng Lei
The high desorption energy barrier for OH– hinders the improvement of the oxygen reduction reaction (ORR) and related devices. Here, an Fe-based atom pair catalyst for ORR is discovered through high-throughput density functional theory calculations. The atomic Te around the Fe1–N4 site (Te1–N2–Fe1–N2) served as an electron pump to achieve charge dilution, contributing to an onset potential of 1.03 V and a half-wave potential of 0.94 V. Moreover, a kinetics current density of 32.4 mA cm–2 and remarkable durability up to 20000 continuous electrolysis cycles (1/4 activity decay that of the Fe1–N4 site) were achieved. An ab initio molecular dynamics simulation revealed the formation process of Fe–Te dual atoms. In situ characterization and comparative experiments verify that the charge dilution toward a single Fe site around atomic Te resulted in promoted O2 conversion and accelerated *OH desorption. The corresponding Al-air batteries showed an open-circuit potential of 1.62 V, a power density of 138.1 mW cm–2, and stable voltages during the long-term discharging process (446 h at 10 mA cm–2 and 270 h at 20 mA cm–2). The study demonstrates the single-atom electron pump as an effective strategy for handling the charge density around single-atom sites for electrocatalysis.
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高影响因子
危险品化学品经营许可证（带存储）