A single-atom Fe–N<sub>4</sub> catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection

Ma, Wenjie; Mao, Junjie; Yang, Xiaoti; Pan, Cong; Chen, Wenxing; Wang, Ming; Yu, Ping; Mao, Lanqun; Li, Yadong

doi:10.1039/c8cc08116f

Cited by 240 publications

(192 citation statements)

References 29 publications

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“…For instance, single‐Fe‐atom catalysts fabricated by pyrolysis approach could not form the homogeneous dispersion in physiological saline and thus hinder their further application in physiological milieu. PEGylated SACs were fabricated by sonicating SACs in an aqueous solution of distearyl phosphatidylethanolamine (DSPE)‐PEG2000, which could serve as reactive oxygen species (ROS) scavengers for protecting cells from oxidative stress …”

Section: Synthetic Strategies Of Sacs For Biomedical Applicationsmentioning

confidence: 99%

Section: Catalytic Activities Of Sacs For Potential Biomedical Applicmentioning

confidence: 99%

“…In addition, a single‐Fe‐atom catalyst, designated as Fe‐SAs/NC, was fabricated by anchoring atomically distributed FeN 4 sites on N‐doped porous carbon (NC) support for mimicking the catalytic activity of catalase (CAT) and superoxide dismutase (SOD) . The CAT‐mimicking capability of Fe‐SAs/NC in decomposing H 2 O 2 into O 2 was investigated by monitoring the production of O 2 using cyclic voltammetry.…”

Section: Catalytic Activities Of Sacs For Potential Biomedical Applicmentioning

confidence: 99%

“…They exhibit high potential in protecting cells from oxidative stress . For instance, Fe single atoms dispersed on N‐doped porous carbon (Fe‐SAs/NC) was fabricated and utilized to mimic antioxidative enzymes for efficiently scavenging ROS . The obtained Fe‐SAs/NC accelerated the disassociation of H 2 O 2 into H 2 O and O 2 as well as O 2 • − into H 2 O 2 and O 2 , thus facilitating them to scavenge cellular ROS as produced in the process of oxidative stress ( Figure a).…”

Section: Biomedical Applications Of Sacsmentioning

confidence: 99%

Section: Biomedical Applications Of Sacsmentioning

confidence: 99%

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Single‐Atom Catalysts in Catalytic Biomedicine

2020

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The intrinsic deficiencies of nanoparticle‐initiated catalysis for biomedical applications promote the fast development of alternative versatile theranostic modalities. The catalytic performance and selectivity are the critical issues that are challenging to be augmented and optimized in biological conditions. Single‐atom catalysts (SACs) featuring atomically dispersed single metal atoms have emerged as one of the most explored catalysts in biomedicine recently due to their preeminent catalytic activity and superior selectivity distinct from their nanosized counterparts. Herein, an overview of the pivotal significance of SACs and some underlying critical issues that need to be addressed is provided, with a specific focus on their versatile biomedical applications. Their fabrication strategies, surface engineering, and structural characterizations are discussed briefly. In particular, the catalytic performance of SACs in triggering some representative catalytic reactions for providing the fundamentals of biomedical use is discussed. A sequence of representative paradigms is summarized on the successful construction of SACs for varied biomedical applications (e.g., cancer treatment, wound disinfection, biosensing, and oxidative‐stress cytoprotection) with an emphasis on uncovering the intrinsic catalytic mechanisms and understanding the underlying structure–performance relationships. Finally, opportunities and challenges faced in the future development of SACs‐triggered catalysis for biomedical use are discussed and outlooked.

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Section: Synthetic Strategies Of Sacs For Biomedical Applicationsmentioning

confidence: 99%

Section: Catalytic Activities Of Sacs For Potential Biomedical Applicmentioning

confidence: 99%

Section: Catalytic Activities Of Sacs For Potential Biomedical Applicmentioning

confidence: 99%

Section: Biomedical Applications Of Sacsmentioning

confidence: 99%

Section: Biomedical Applications Of Sacsmentioning

confidence: 99%

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Single‐Atom Catalysts in Catalytic Biomedicine

2020

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Heme Cofactor‐Resembling Fe–N Single Site Embedded Graphene as Nanozymes to Selectively Detect H₂O₂ with High Sensitivity

Kim

Lee

Kim

et al. 2019

Adv Funct Materials

210

116

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Over the past decade, the catalytic activity of nanozymes has been greatly enhanced, but their selectivity is still low and considered a critical issue to overcome. Herein, Fe–N4 single site embedded graphene (Fe–N‐rGO), which resembles the heme cofactor present in natural horseradish peroxidase, shows a marked enhancement in peroxidase‐like catalytic efficiency of up to ≈700‐fold higher than that of undoped rGO as well as excellent selectivity toward target H2O2 without any oxidizing activity. Importantly, when Fe or N is doped alone or when Fe is replaced with another transition metal in the Fe–N4 site, the activity is negligibly enhanced, showing that mimicking the essential cofactor structure of natural enzyme might be essential to design the catalytic features of nanozymes. Density functional theory results for the change in Gibbs free energy during the peroxide decomposition reaction explain the high catalytic activity of Fe–N‐rGO. Based on the high and selective peroxidase‐like activity of Fe–N‐rGO, trace amounts of H2O2 produced from the enzymatic reactions from acetylcholine and cancerous cells are successfully quantified with high sensitivity and selectivity. This work is expected to encourage studies on the rational design of nanozymes pursuing the active site structure of natural enzymes.

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A Nanozyme‐Based Artificial Peroxisome Ameliorates Hyperuricemia and Ischemic Stroke

Zhang

Wang

et al. 2020

Adv Funct Materials

167

104

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Artificial peroxisome has drawn a lot of attentions for its usefulness in fabricating protocell system and great potential in treating diseases. However, it is still a significant challenge to prepare a practicable artificial peroxisome to complement multiple and stable functions under physiological condition. Herein, a novel strategy is reported to design an artificial peroxisome using a nanozyme to accommodate multiple enzyme‐like activities that mimics those enzymes in natural peroxisome. The enzymatic active sites are introduced into graphitized moieties on the shell of a hollow carbon nanozyme by doping iron and nitrogen to form Fe–N4 coordination and atomic Fe cluster. With Fe clusters as reversible cofactors and Fe–N4 as prosthetic group, the resulted carbon nanozyme exhibits stable and multiple peroxisomal‐like activities, including catalase, uricase, superoxide dismutase, peroxidase, and oxidase, which is referred as nanozyme‐based artificial peroxisome (pero‐nanozysome). This pero‐nanozysome shows therapeutic effect for treating hyperuricemia and protecting neurons from free radicals generated during ischemic stroke by employing the tandem activities of uricase‐catalase and superoxide‐dismutase‐catalase, respectively. This study indicates that the pero‐nanozysome is a promising candidate to design artificial peroxisome performing in vivo functions.

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A single-atom Fe–N₄ catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection

Abstract: Single-atom catalysts can serve as single-atom-based enzymes (SAzymes) with multi-antioxidative activities for reactive oxygen species scavenging.

Cited by 240 publications

References 29 publications

Single‐Atom Catalysts in Catalytic Biomedicine

Single‐Atom Catalysts in Catalytic Biomedicine

Heme Cofactor‐Resembling Fe–N Single Site Embedded Graphene as Nanozymes to Selectively Detect H₂O₂ with High Sensitivity

A Nanozyme‐Based Artificial Peroxisome Ameliorates Hyperuricemia and Ischemic Stroke

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A single-atom Fe–N4 catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection

Abstract: Single-atom catalysts can serve as single-atom-based enzymes (SAzymes) with multi-antioxidative activities for reactive oxygen species scavenging.

Cited by 240 publications

References 29 publications

Single‐Atom Catalysts in Catalytic Biomedicine

Single‐Atom Catalysts in Catalytic Biomedicine

Heme Cofactor‐Resembling Fe–N Single Site Embedded Graphene as Nanozymes to Selectively Detect H2O2 with High Sensitivity

A Nanozyme‐Based Artificial Peroxisome Ameliorates Hyperuricemia and Ischemic Stroke

Contact Info

Product

Resources

About

A single-atom Fe–N₄ catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection

Heme Cofactor‐Resembling Fe–N Single Site Embedded Graphene as Nanozymes to Selectively Detect H₂O₂ with High Sensitivity