Creating peroxidase-mimetic clusterzymes for efficient and selectively enzymatic diagnosis of biomarkers

Zhu, Huang; Deng, Jiuhong; Mu, Shengdong; Xiao, Sutong; Li, Qian; Wang, Weiwen; Gao, Yang; Luο, Xingguang; Gao, Shanshan; Cheng, Chong

doi:10.1016/j.cej.2023.142215

Cited by 13 publications

(4 citation statements)

References 64 publications

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“…In the presence of H 2 O 2 , FePorNW‐DAP can efficiently catalyze the oxidation of 3,3′,5,5′‐tetramethylbenzidine (TMB) to form the blue‐colored oxidized‐TMB with a characteristic absorbance of 652 nm, whereas the bare PorNW exhibits almost no activity (Figure 4b). [ 51 ] Then, 5,5‐dimethyl‐1‐pyrroline N‐oxide (DMPO) as the specific spin trap reagent was used to verify the type of free radical products has been determined through electron spin resonance (ESR), which results show significant •OH signals (Figure 4c). In addition, the •OH generation of FePorNW‐DAP has also been confirmed by using the terephthalic acid (TA) assay (Figure 4d).…”

Section: Resultsmentioning

confidence: 99%

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Wang,

Li,

Zhao

et al. 2023

Adv Funct Materials

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Constructing highly effective sonosensitizers that integrate tumor microenvironment (TME)‐adaptive and ultrasound (US)‐controllable production of reactive oxygen species (ROS) to amplify tumor immunotherapies is extremely desirable but remains challenging. Here, inspired by the coordination structure and biocatalytic effects of Fe‐based peroxidase, a dual‐functional artificial peroxidase is synthesized with ferriporphyrin networks (FePorNW‐DAP) to serve a TME‐adaptive and US‐controllable ROS‐generator for amplifying tumor immunotherapies in breast cancer via immunogenic cell death. Owing to the structural advantages of the ferriporphyrin‐based large d–π‐conjugated networks with the monatomic Fe─N4 coordination center, moderate interaction with H2O2, and decreased bandgap, the FePorNW‐DAP displays efficient dual‐functional ROS production capabilities to combat tumor cells and amplify the tumor immunotherapies, 1) utilize locally produced H2O2 in the TME to catalytically generate potent •OH and other ROS species; simultaneously, 2) external US irradiation can further boost the generation of •OH and 1O2. This work provides not only critical evidence that the proposed dual‐functional artificial peroxidases can induce a strong antitumor immune response and immune memory but also offers essential guidance for creating a high‐performance and biocompatible strategy to regulate the immunosuppression TME and enhance the antitumor immune responses of breast cancer.

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Section: Resultsmentioning

confidence: 99%

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Wang,

Li,

Zhao

et al. 2023

Adv Funct Materials

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“…This could be further verified by the atomic elemental mapping images in Figure 3i,l; it shows abundant mesopore defects and probably increases the exposure of active sites in DW-CAB. [40][41][42] Moreover, it is well-established that the magnitude of the ligand loss is related with the defectivity of MOFs. [43,44] Thermogravimetric analysis (TGA)-differential scanning calorimetry (DSC) simultaneous thermal analysis shows that the residue >600 °C is pure ZnO.…”

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Engineering Zinc–Organic Frameworks‐Based Artificial Carbonic Anhydrase with Ultrafast Biomimetic Centers for Efficient Hydration Reactions

Li,

Xu,

et al. 2023

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Constructing effective and robust biocatalysts with carbonic anhydrase (CA)‐mimetic activities offers an alternative and promising pathway for diverse CO2‐related catalytic applications. However, there is very limited success has been achieved in controllably synthesizing CA‐mimetic biocatalysts. Here, inspired by the 3D coordination environments of CAs, this study reports on the design of an ultrafast ZnN3‐OH2 center via tuning the 3D coordination structures and mesoporous defects in a zinc–dipyrazolate framework to serve as new, efficient, and robust CA‐mimetic biocatalysts (CABs) to catalyze the hydration reactions. Owing to the structural advantages and high similarity with the active center of natural CAs, the double‐walled CAB with mesoporous defects displays superior CA‐like reaction kinetics in p‐NPA hydrolysis (V0 = 445.16 nM s−1, Vmax = 3.83 µM s−1, turnover number: 5.97 × 10−3 s−1), which surpasses the by‐far‐reported metal–organic frameworks‐based biocatalysts. This work offers essential guidance in tuning 3D coordination environments in artificial enzymes and proposes a new strategy to create high‐performance CA‐mimetic biocatalysts for broad applications, such as CO2 hydration/capture, CO2 sensing, and abundant hydrolytic reactions.

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“…29 On the other hand, horseradish peroxidase (HRP) is a catalyzing enzyme that can detect H 2 O 2 , and its activity on the electrode directly affects the performance of electrochemical biosensors. 30,31 Unfortunately, the poor stability and inherent fragility of HRP result in high cost and limited applications when employed in electrochemical biosensors. 32 An effective approach to HRP immobilization is one of the key issues determining the performance of detection devices for H 2 O 2 .…”

Section: Introductionmentioning

confidence: 99%

Multi-MXene assisted large-scale manufacturing of electrochemical biosensors based on enzyme-nanoflower enhanced electrodes for the detection of H₂O₂ secreted from live cancer cells

Wang,

Ma,

Shao

et al. 2024

Nanoscale

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Creating peroxidase-mimetic clusterzymes for efficient and selectively enzymatic diagnosis of biomarkers

Cited by 13 publications

References 64 publications

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Engineering Zinc–Organic Frameworks‐Based Artificial Carbonic Anhydrase with Ultrafast Biomimetic Centers for Efficient Hydration Reactions

Multi-MXene assisted large-scale manufacturing of electrochemical biosensors based on enzyme-nanoflower enhanced electrodes for the detection of H₂O₂ secreted from live cancer cells

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Creating peroxidase-mimetic clusterzymes for efficient and selectively enzymatic diagnosis of biomarkers

Cited by 13 publications

References 64 publications

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Dual‐Functional Artificial Peroxidases with Ferriporphyrin Centers for Amplifying Tumor Immunotherapies via Immunogenic Cell Death

Engineering Zinc–Organic Frameworks‐Based Artificial Carbonic Anhydrase with Ultrafast Biomimetic Centers for Efficient Hydration Reactions

Multi-MXene assisted large-scale manufacturing of electrochemical biosensors based on enzyme-nanoflower enhanced electrodes for the detection of H2O2 secreted from live cancer cells

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Product

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Multi-MXene assisted large-scale manufacturing of electrochemical biosensors based on enzyme-nanoflower enhanced electrodes for the detection of H₂O₂ secreted from live cancer cells