Hedgehog artificial macrophage with atomic-catalytic centers to combat Drug-resistant bacteria

Long, Yanping; Li, Ling; Xu, Tao; Wu, Xizheng; Gao, Yun; Huang, Jianbo; He, Chao; Ma, Tian; Ma, Lang; Cheng, Chong; Zhao, Changsheng

doi:10.1038/s41467-021-26456-9

Cited by 121 publications

(81 citation statements)

References 48 publications

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“…Pathogenic drug-resistant bacteria have displayed enormous threaten human life, engineering more effective ROS-based strategies for inhibiting drug-resistant bacteria shows essential importance in next-generation nanomedicines. [6,46,47] After revealing the outstanding ROS-catalytic properties of the electronic structure modulated VO x -AE; to show their application potential, we then carefully examine its activity in combating drug-resistant bacteria by taking the methicillin-resistant Staphylococcus aureus (MRSA) as a representative. [48] We first perform the minimal bactericidal concentration (MBC) tests by the classical plate count method to quantitatively analyze the bacterial viability (Figure 6a).…”

Section: Resultsmentioning

confidence: 99%

Modulating Electron Transfer in Vanadium‐Based Artificial Enzymes for Enhanced ROS‐Catalysis and Disinfection

Cao

et al. 2022

Advanced Materials

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The dramatically increasing demands in enzyme-like catalytic biosynthesis and biotherapeutics have promoted thrilling innovations to engineer artificial enzymes (AEs), [1][2][3][4][5][6][7][8] especially the haloperoxidase (HPO)-like AEs that can generate potent reactive oxygen species (ROS), [9][10][11][12] including • OH, • O 2 -, and HClO/HBrO, for antibacterial and antitumor applications. [13][14][15][16][17][18][19][20][21] Despite the fast flourishment of HPO-like AEs, further enhancing their biocatalytic performances is still a confusing black box since their electronic structures of metal centers and ROScatalytic mechanisms remain largely unclear. [22] The grand challenge is to develop new ideas and precise theoretical guidance for the de novo design of HPOlike AEs and clarify the corresponding electronic structures and catalytic behaviors of metal centers. [23,24] In particular, the vanadium oxide (V 2 O 5 ) is one of the most representative nanomaterials that displays HPO-like activities, which shows broad application potentials from killing pathogenic cells to preventing marine biofouling by catalyzing H 2 O 2 to potent ROS. Compared to natural HPO, the V 2 O 5 -based AEs provide a costeffective, stable, and broad reaction condition pathway. However, the currently reported strategies, [25,26] such as size tuning, modification of composition, and crystal facets engineering, present limited effects on further enhancing the biocatalytic performances of V 2 O 5 -based AEs. Pathways that can efficiently augment the intrinsic ROS-catalytic activities of metal centers in V 2 O 5 -based AEs are still missing.In V 2 O 5 -based AEs, the V centers possess depressed d electrons density due to its coordination with neighboring electronegative oxygen atoms, [27,28] which causes the V-d 2 z electrons (this d 2 z orbital is perpendicular to the basal plane) to become more accessible to form head-on-head sigma bonds with O-p z orbital. Therefore, the V centers in V 2 O 5 possess strong interaction with H 2 O 2 and suppressed dissociation of oxygenintermediates, [25] consequently resulting in reduced reaction dynamics. The de novo design of the d electrons of V centers to modulate the adsorption-energy between the H 2 O 2 and metal sites is essential for further enhancing their intrinsic ROS-catalytic activities. [29] One approach to weaken the accessibility of d 2 z electrons of metal centers is the filling of d yz orbitals near Nanomaterials-based artificial enzymes (AEs) have flourished for more than a decade. However, it is still challenging to further enhance their biocatalytic performances due to the limited strategies to tune the electronic structures of active centers. Here, a new path is reported for the de novo design of the d electrons of active centers by modulating the electron transfer in vanadium-based AEs (VO x -AE) via a unique Zn-O-V bridge for efficient reactive oxygen species (ROS)-catalysis. Benefiting from the electron transfer from Zn to V, the V site in VO x -AE exhibits a lower valence state tha...

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Section: Resultsmentioning

confidence: 99%

Modulating Electron Transfer in Vanadium‐Based Artificial Enzymes for Enhanced ROS‐Catalysis and Disinfection

Cao

et al. 2022

Advanced Materials

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“…The sterilization tests of TCNCoT were evaluated according to a previous method with slight modifications [22] . All the glassware and culture medium solution were autoclaved at 121 °C for 30 min before the microbiological experiments [23] .…”

Section: Methodsmentioning

confidence: 99%

COVID-19-inspired “artificial virus” to combat drug-resistant bacteria by membrane-intercalation- photothermal-photodynamic multistage effects

Wang²,

Wang³

et al. 2022

Chemical Engineering Journal

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“…The versatility of transition metal electronic states and coordination modes lays the foundation for transition metal catalysis in chemistry, which also provides opportunities to develop new AMEs starting from nature's vast collection of metalloproteins. [5][6][7][8] Since the ferromagnetic nanoparticles were reported with peroxidase (POD)mimetic activity, [9] a lot of metalnanomaterialbased AMEs, exhibiting biocatalytic activities of oxidase (OXD), [10,11] POD, [12] halogen peroxidase (HPO), [13] etc., have been discovered, [8,[14][15][16] among which, the metalNcoordinated centers supported by carbo naceous substrates have emerged as promising candidates to engineer AMEs to mimic the biocatalytic effects of their natural counterparts. [16][17][18][19][20][21] However, their catalytic activities, substrates' selectivities, kinetics, and reactive oxygen species (ROS) products have not been investigated since the synthesis of AMEs that consist of different atomic metalN centers but exhibit similar physicochemical and coordination structures remains a substantial challenge.…”

Section: Introductionmentioning

confidence: 99%

A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

et al. 2022

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MetalN-coordinated centers supported by carbonaceous substrates have emerged as promising artificial metalloenzymes (AMEs) to mimic the biocatalytic effects of their natural counterparts. However, the synthesis of well-defined AMEs that contain different atomic metalN centers but present similar physicochemical and coordination structures remains a substantial challenge. Here, 20 different types of AMEs with similar geometries and welldefined atomic metalN-coordinated centers are synthesized to compare and disclose the catalytic activities, substrate selectivities, kinetics, and reactive oxygen species (ROS) products. Their oxidase (OXD)-, peroxidase (POD)-, and halogen peroxidase (HPO)-mimetic catalytic behaviors are systematically explored. The Fe-AME shows the highest OXD-and HPO-mimetic activities compared to the other AMEs due to its high v max (0.927 × 10 −6 m s −1 ) and low K m (1.070 × 10 −3 m), while the Cu-AME displays the best POD-like performance. Furthermore, theoretical calculation reveals that the ROS-catalytic paths and activities are highly related to the electronic structures of the metal centers. Benefiting from its facile adsorption of H 2 O 2 molecule and lower energy barrier to generating •O 2 − , the Fe-AME displays higher ROS-catalytic performances than the Mn-AME. The engineered AMEs show not only remarkably high ROS-catalytic performances but also provide new guidance toward developing metalN-coordinated biocatalysts for broad application fields.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202200255.

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Hedgehog artificial macrophage with atomic-catalytic centers to combat Drug-resistant bacteria

Cited by 121 publications

References 48 publications

Modulating Electron Transfer in Vanadium‐Based Artificial Enzymes for Enhanced ROS‐Catalysis and Disinfection

Modulating Electron Transfer in Vanadium‐Based Artificial Enzymes for Enhanced ROS‐Catalysis and Disinfection

COVID-19-inspired “artificial virus” to combat drug-resistant bacteria by membrane-intercalation- photothermal-photodynamic multistage effects

A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers

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