ANALYTICA CHIMICA ACTA
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2025
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IF 6
Rong Huang,Zhong Dong,Wanyi Zhang,Zhenggang Xue,Dongmei Deng,Wei Wang,Yuanyuan Li,Haibo He,Liqiang Luo
Background Organophosphorus pesticides contamination significantly threatens the ecological environment. Therefore, developing sensitive and efficient point-of-care detection methods is essential. Results In this work, Cu−N 4 single-atom nanozymes on nitrogen-doped carbon (Cu SAs/NC) with dual enzyme-mimicking activities (peroxidase-like and oxidase-like) were prepared for point-of-care detection of parathion using acetylcholinesterase inhibition-based colorimetric sensing mechanism. Cu SAs/NC shows high catalytic activity with high turnover number (K cat ) of ∼24.07 min −1 and K cat /K m of ∼1.35×10 5 M −1 min −1 . Experimental findings in combination with density functional theory simulations demonstrate that Cu centers in Cu SAs/NC play a pivotal role in intermediate binding optimization, which contributes to a decreased reaction energy barrier. Hence, a colorimetric sensing platform based on Cu SAs/NC was constructed for point-of-care detection of parathion, achieving a detection limit of 0.79 ng mL −1 . Significance This study provides a novel strategy for structuring single-atom nanozymes with enhanced enzyme-mimicking activity, showing great promise for advanced environmental protection.
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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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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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Advanced Science
·
2026
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IF 14.1
Daohu Sheng,Siyao Cheng,Mengmeng Zhang,Jinglei Zhang,Xufei Zhu,Weijin Li,Bo Zhang,Aming Xie
The dielectric response of carbon-based single-atom (SA) absorbers is intrinsically constrained by the highly symmetric charge distribution of planar M-N 4 coordination motifs, which suppresses dipole polarization and limits electromagnetic wave (EMW) attenuation. Here, a nanocurvature-driven symmetry-breaking strategy is proposed to activate latent dielectric polarization at SA sites through geometric regulation. By combining click chemistry with template-assisted synthesis, metal SAs are anchored onto hollow nitrogen-doped carbon spheres with precisely tunable diameters, enabling systematic modulation of local nanocurvature. Theoretical calculations and experimental analyses reveal that curvature-induced surface charge accumulation disrupts the electronic symmetry at Ni-N 4 centers, markedly enhancing local charge density, dipole moments, and polarizability. Consequently, the optimized Ni/HNC-200 absorber achieves an ultralow minimum reflection loss of −74.1 dB, representing a staggering 390% enhancement over HNC-200 (−15.1 dB), and exhibits a reduced radar cross section of −70.49 dB m 2 . A flexible electronic patch further demonstrates over fivefold suppression of electric-field radiation from mobile phone chips. The universality of this mechanism is validated in Co- and Cu-based systems, establishing nanocurvature as a geometry-enabled design paradigm for high-performance SAs EMW absorbers.
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NUCLEIC ACIDS RESEARCH
·
2025
·Vol. 53
·期 10
·
IF 13.1
Wang Qi,Du Yuhao,Yan Shen,Lu Ziang,Tang Yongling,Xiao Feng,Zhou Fuling,Zhou Xiang
N4-Acetylcytidine (ac4C) is an emerging epitranscriptomic mark involved in regulating RNA stability, translation, and gene expression. Despite its emerging role in gene regulation and disease, current methods for in situ detection of ac4C-modified RNA lack sensitivity and specificity. To overcome these challenges, we developed fluorine metabolic labeling mediated proximity ligation assay (FMPLA), a method combining fluorine-based metabolic labeling with a proximity ligation assay for precise detection of newly synthesized fluoro-metabolically labeled ac4C sites. This approach enables high-sensitivity visualization of multiple RNA species, and provides insights into the abundance and spatial dynamics of ac4C-modified RNAs during the cell cycle and under chemotherapeutic stress. Additionally, FMPLA reveals distinct RNA modification patterns in drug-resistant cancer cells, highlighting its potential in studying functions and mechanisms of RNA ac4C modification.
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JACS Au
·
2024
·
IF 8.5
Xixi Liu,Liang Huang,Yurong He,Peng Zhou,Xuedan Song,Zehui Zhang
It remains challenging to construct C═N bonds due to their facile hydrogenation. Herein, a single Co atom catalyst was discovered to be active for the selective construction of C═N bonds toward the synthesis of imines and N-heterocycles via reductive coupling of nitroarenes with various alcohols, including inert aliphatic ones. DFT calculations and experimental data revealed that the transfer hydrogenation proceeded via the intramolecular hydride transfer and the transfer of H from the α-Csp3-H bond to the nitro group was the rate-determining step. The single Co atoms served as a bridge to transfer the electrons from the catalyst to the adsorbed alcohol molecules, resulting in the activation of the α-Csp3-H bond. Unlike metal nanoparticles, the C═N bonds in imine products can be reserved due to the large steric hindrance from substituents on C and N. DFT calculation also confirmed that transfer hydrogenation of the C═N bonds in imines is thermodynamically unfavored with a much higher energy barrier compared with the transfer hydrogenation of the –NO2 group (1.47 vs 1.15 eV).
研究领域:
化学
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催化反应
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理论计算
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Shao-Qi Zhi,Jun-Yuan Zhang,Song-Hai Wu,Wen-Shuang Zhu,Yu-Dong Shan,Yong Liu,Xu Han
Turning aromatic sulfur impurities to value-added polymers is a promising technology for fuel desulfurization. In this study, Cu(I,II)@g-C3N4 plates prepared via facile calcination show high reactivity in catalytic oxidation of benzothiophene (BT) by persulfate in a mixture of MeCN/H2O (v/v = 50/50). Quenching experiments rule out the primary contributions of SO4•–, •OH, and O2•– to BT oxidation and confirm the presence of carbon-centered radicals during the desulfurization process. XPS and Raman analyses reveal that Cu(I) and graphitic-N are reactive sites for persulfate activation, accompanied with moderate activation of the peroxo group in persulfate via the nonradical pathway. Solid characterizations indicate the formation of polybenzothiophene S,S-dioxide during the oxidation process, which further reveals that the moderately activated persulfate abstracts H from BT to form a BT radical cation, followed by subsequent polymerization of BT radical cations to a BT tetramer, and then the BT tetramer is further oxidized to a BT S,S-dioxide tetramer. The high electrochemical stability and pseudo-capacitive properties of the obtained polymers also imply their high potential to be used for capacitors. This work provides new insight on turning aromatic sulfur impurities in fuels to “treasures”.
研究领域:
化学工程
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环境科学
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INORGANIC CHEMISTRY COMMUNICATIONS
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2024
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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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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.3
Geng Zhang,Bolong Jiang,Decheng Lu,Xueqin Wang,Yuanyuan Wang,Hua Song
The sluggish kinetics of the oxygen reduction reaction (ORR) at the cathode severely limits the electricity generation and pollutant degradation of microbial fuel cells (MFCs). Herein, we report a facile one-pot pyrolysis strategy for fabricating a highly dispersed iron-embedded N/S co-doped hierarchical porous carbon catalyst (FeSNC) with accessible Fe−N 4 −S active sites using tetramethylammonium hydroxide (TMAH)-optimized Fe-ZIF-8-N-H precursors. TMAH enables rapid synthesis (16 min), 3.6-fold yield enhancement, mesopore engineering for efficient Fe 2+ capture and dense Fe−N 4 −S site formation, and hierarchical pore construction for accelerated mass/electron transport. The Fe source (NH 4 ) 2 Fe(SO 4 ) 2 ·6 H₂O synchronously introduces N and S to optimize pyridinic N and Fe−N x coordination. Theoretical calculations reveal that S-doping modulates the electronic structure of the central Fe, while mesopore-induced defects act as a secondary modulator, collectively establishing a dual-modulation mechanism to optimize the adsorption/desorption of ORR intermediates. The 6 %FeSNC-N-H catalyst outperforms commercial Pt/C in ORR across neutral/alkaline/acidic media and, as an MFC cathode, delivers a peak power density of 987.0 ± 5.3 mW cm⁻², 96.75 % COD removal, and high degradation efficiency for phenol (93.4 %) and methylene blue (95.6 %). This work underscores the critical synergy between of metal centers electronic microenvironment and nanostructural pore engineering for advanced electrocatalysts.
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Nanomaterials
·
2026
·Vol. 16
·期 13
·813
·
IF 4.8
Manman Zou,Xiaoling Zhuang,Qin Tian,Jili Yuan
Two-electron oxygen reduction reaction (2e−-ORR) represents a sustainable and energy-efficient approach for decentralized hydrogen peroxide (H2O2) production compared with the conventional anthraquinone process. Among various electrocatalysts, metal–nitrogen–carbon (M–N–C) materials have attracted extensive attention owing to their tunable electronic structures and favorable *OOH adsorption behavior. However, the uncontrolled pyrolysis process generally leads to structurally heterogeneous and ill-defined coordination environments, making it difficult to precisely regulate active sites and understand catalytic mechanisms. Herein, we report a single-atom catalyst (CoN@OCNT) featuring spatially confined pyridinic-N-coordinated Co single sites, synthesized by anchoring a well-defined hexapod terpyridine Co-precursor onto oxidized carbon nanotubes (OCNTs) to suppress metal aggregation during pyrolysis. Benefiting from the optimized coordination environment and enhanced mass/electron transfer, the CoN@OCNT catalyst exhibits nearly 100% H2O2selectivity over a wide potential window from −1.0 to 0.66 V versus RHE in neutral electrolyte. In situ FT-IR and Raman spectroscopy reveal a rapid *OOH-mediated reaction pathway during the 2e−-ORR process. Furthermore, membrane electrode assembly (MEA) testing demonstrates an H2O2production rate of 21.8 mol h−1gcat−1with stable operation over 80 h at 60 mA cm−2. Remarkably, at an industrially relevant current density of 300 mA cm−2, the catalyst achieves a record H2O2production rate of 70.3 mol h−1gcat−1and a salt-free H2O2concentration of 9.4 mM, highlighting its great potential for practical large-scale H2O2electrosynthesis in neutral media.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Shu-Hu Yin,Xiao-Yang Cheng,Yu Han,Ting Zhu,Zhong-Wei Yu,Rui Huang,Jun Xu,Yan-Xia Jiang,Shi-Gang Sun
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N 4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe–N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential ( E 1/2 ) of 0.840 V and peak power density ( P max ) of 938 mW cm –2 under 150 kPa absolute H 2 -O 2 . These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E 1/2 and +42% in P max ). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E 1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N 4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site –1 s –1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1–2 orders of magnitude (< 1 e site –1 s –1 ); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
研究领域:
催化化学
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材料科学
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电化学
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能源材料
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表面科学
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纳米催化
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质子交换膜燃料电池
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Fancang Meng,Huan Wu,Boyu Jia,Kexiang Li,Zhihua Wang,He Zhu,Chao Chen,Qingmin Ji
The development of Fe-N-C electrocatalysts for the oxygen reduction reaction (ORR) is crucial for sustainable energy technologies, yet achieving a high density of atomically dispersed Fe-Nx sites remains a challenge. Herein, we proposed a novel spatial confinement strategy based on the molecular-level infiltration of iron-coordinated, water-soluble fullerene (Fe/wsC60) into self-assembled fullerene microbelts (FMB). The -NH2/-OH functionalized C60s act as molecular metal chelator and nitrogen source, while the flexible FMB framework facilitates their effective permeation. This nanoscale confinement effectively mitigates Fe aggregation during pyrolysis, yielding a catalyst with abundant atomically dispersed curved Fe-N4 sites alongside fine Fe3C nanoparticles. The resultant (Fe/N@FMB) catalyst demonstrates an exceptional ORR activity and stability in alkaline media with a half-wave potential of 0.891 V, surpassing Pt/C and control samples derived solely from wsC60 or FMB. When integrated into a zinc-air battery, it also achieves a higher open-circuit voltage and power density than Pt/C. Theoretical calculations reveal that the curved carbon matrix and adjacent Fe3C synergistically modulate the electronic structure of the Fe-N4 moiety, thereby boosting the ORR kinetics. This work highlights the importance of nanoscale architectural design for precise precursor confinement in developing advanced electrocatalysts.
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