N, P, S Codoped Carbon Nanozymes with Enhanced Peroxidase-like Activity and Binding Affinity for Total Antioxidant Capacity Assay

Wang, Yingsha; Feng, Qinghua; Liu, Meili; Xue, Liuheng; Wang, Gang; Zhang, Shouting; Hu, Wenping

doi:10.1021/acsanm.3c04650

Cited by 12 publications

(2 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…To explore the geometric and electronic structure of heteroatom (P, S, B, and N) doping Fe–N configurations, a 6 × 6 × 1 N-doped carbon layer with an Fe atom anchored on the N 4 vacancy is built to model the Fe–N 4 –C structure (Figure a). According to previous studies, ,,− ,− both coordinating N and neighboring C atoms around the central Fe are the sites that can be doped, and the blue area inside the dashed box in Figure a is chosen as the doping region for heteroatoms. To eliminate the interaction between atoms in adjacent periodic layers, a vacuum layer of up to 15 Å is added to the surface of the N-doped carbon layer along the z direction.…”

Section: Computational Models and Methodsmentioning

confidence: 99%

“…Fe Fer –SAC with four coordinating N atoms has highest POD-like catalytic activity among the three Fe SACs due to the lower OH generation barrier . And the FeN 5 with axial N coordination exhibits superior POD/OXD (oxidase)-like activity owing to a clear electron push effect. , In a word, the atomic radius, electronegativity, doping ratio, and doping position of different heteroatoms are crucial factors influencing catalytic activity and selectivity. , However, most theoretical studies focus on only one or two of these aspects and most analyses are based on experimental results, while a comprehensive and in-depth study of doping factors for the binding affinity of H 2 O 2 linked to POD-like activity at the theoretical level is lacking.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Nonmetal Doping Modulates Fe Single-Atom Catalysts for Enhancement in Peroxidase Mimicking via Symmetry Disruption, Distortion, and Charge Transfer

Liu,

Sun,

et al. 2024

ACS Omega

View full text Add to dashboard Cite

Developing biomimetic catalysts with excellent peroxidase (POD)-like activity has been a long-standing goal for researchers. Doping nonmetallic atoms with different electronegativity to boost the POD-like activity of Fe−N−C single-atom catalysts (SACs) has been successfully realized. However, the introduction of heteroatoms to regulate the coordination environment of the central Fe atom and thus influence the activation of the H 2 O 2 molecule in the POD-like reaction has not been extensively explored. Herein, the effect of different doping sites and numbers of heteroatoms (P, S, B, and N) on the adsorption and activation of H 2 O 2 molecules of Fe−N sites is thoroughly investigated by density functional theory (DFT) calculations. In general, alternation in the catalytic efficiency directly depends on the transfer of electrons and the geometrical shifts near the Fe−N site. First, the symmetry disruption of the Fe−N 4 site by P, S, and B doping is beneficial to the activation of H 2 O 2 due to a significant reduction in the adsorption energies. In some cases, without Fe−N 4 site disruption, the configurations fail to modulate the adsorption behavior of H 2 O 2 . Second, Fe−N−P/S configurations exhibit a stronger affinity for H 2 O 2 molecules due to the significant out-of-plane distortions induced by larger atomic radii of P and S. Moreover, the synergistic effects of Fe and doping atoms P, S, and B with weaker electronegativity than that of N atoms promote electron donation to generated oxygencontaining intermediates, thus facilitating subsequent electron transfer with other substrates. This work demonstrates the critical role of tuning the coordinating environment of Fe−N active centers by heteroatom doping and provides theoretical guidance for controlling the types by breaking the symmetry of SACs to achieve optimal POD-like catalytic activity and selectivity.

show abstract

Section: Computational Models and Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Nonmetal Doping Modulates Fe Single-Atom Catalysts for Enhancement in Peroxidase Mimicking via Symmetry Disruption, Distortion, and Charge Transfer

Liu,

Sun,

et al. 2024

ACS Omega

View full text Add to dashboard Cite

show abstract

Fine‐Tuning Electron Transfer for Nanozyme Design

Zong,

Xu,

Pang

et al. 2024

Adv Healthcare Materials

View full text Add to dashboard Cite

Nanozymes, with their versatile composition and structural adaptability, present distinct advantages over natural enzymes including heightened stability, customizable catalytic activity, cost‐effectiveness, and simplified synthesis process, making them as promising alternatives in various applications. Recent advancements in nanozyme research have shifted focus from serendipitous discovery toward a more systematic approach, leveraging machine learning, theoretical calculations, and mechanistic explorations to engineer nanomaterial structures with tailored catalytic functions. Despite its pivotal role, electron transfer, a fundamental process in catalysis, has often been overlooked in previous reviews. This review comprehensively summarizes recent strategies for modulating electron transfer processes to fine‐tune the catalytic activity and specificity of nanozymes, including electron‐hole separation and carrier transfer. Furthermore, the bioapplications of these engineered nanozymes, including antimicrobial treatments, cancer therapy, and biosensing are also introduced. Ultimately, this review aims to offer invaluable insights for the design and synthesis of nanozymes with enhanced performance, thereby advancing the field of nanozyme research.

show abstract

Carbon-based nanozymes: design, catalytic mechanisms, and environmental applications

Zhuang,

Yu,

Dong

et al. 2024

Anal Bioanal Chem

View full text Add to dashboard Cite

N, P, S Codoped Carbon Nanozymes with Enhanced Peroxidase-like Activity and Binding Affinity for Total Antioxidant Capacity Assay

Cited by 12 publications

References 50 publications

Nonmetal Doping Modulates Fe Single-Atom Catalysts for Enhancement in Peroxidase Mimicking via Symmetry Disruption, Distortion, and Charge Transfer

Nonmetal Doping Modulates Fe Single-Atom Catalysts for Enhancement in Peroxidase Mimicking via Symmetry Disruption, Distortion, and Charge Transfer

Fine‐Tuning Electron Transfer for Nanozyme Design

Carbon-based nanozymes: design, catalytic mechanisms, and environmental applications

Contact Info

Product

Resources

About