A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers (Adv. Mater. 16/2022)

Cao, Sujiao; Zhao, Zhenyang; Zheng, Yijuan; Wu, Zihe; Ma, Tian; Zhu, Bihui; Yang, Chengdong; Xiang, Xi; Ma, Lang; Han, Xianglong; Wang, Yi; Guo, Quanyi; Qiu, Li; Cheng, Chong

doi:10.1002/adma.202270120

Cited by 18 publications

(25 citation statements)

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“…As one of the essential antioxidant natural metalloenzymes, CAT composes of FeN active sites coordinated to the porphyrin macrocycle (Figure 1a). [17,[20][21][22] However, the arbitrarily prepared FeN coordination structure usually shows barely any or very low CAT-like activities (Figure S1, Supporting Information); this activity difference may be attributed to the lack of 3D spatial configuration or coordination structure as that of CAT. It has been reported that modulating the metal Exploring high-efficiency reactive oxygen species (ROS)-elimination materials is of great importance for combating oxidative stress in diverse diseases, especially stem-cell-based biotherapeutics.…”

Section: Introductionmentioning

confidence: 99%

Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Sun

Xing

et al. 2022

Advanced Materials

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Exploring high‐efficiency reactive oxygen species (ROS)‐elimination materials is of great importance for combating oxidative stress in diverse diseases, especially stem‐cell‐based biotherapeutics. By mimicking the FeN active centers of natural catalase, here, an innovative concept to design ROS‐elimination artificial biocatalysts with Ru catalytic centers for stem‐cell protection is reported. The experimental studies and theoretical calculations have systematically disclosed the activity merits and structure diversities of different Ru sites when serving as ROS‐elimination artificial biocatalysts. Benefiting from the metallic electronic structures and synergetic effects of multiple sites, the artificial biocatalysts with Ru cluster centers present exceptional ROS‐elimination activity; notably, it shows much higher catalytic efficiency per Ru atom on decomposing H2O2 when compared to the isolated single‐atom Ru sites, which is more efficient than that of the natural antioxidants and recently reported state‐of‐the‐art ROS‐scavenging biocatalysts. The systematic stem‐cell protection studies reveal that the catalase‐like artificial biocatalysts can provide efficient rescue ability for survival, adhesion, and differentiation functions of human mesenchymal stem cells in high ROS level conditions. It is suggested that applying these artificial biocatalysts with Ru cluster centers will offer a new pathway for engineering high‐performance ROS‐scavenging materials in stem‐cell‐based therapeutics and many other ROS‐related diseases.

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Section: Introductionmentioning

confidence: 99%

Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Sun

Xing

et al. 2022

Advanced Materials

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“…The high-resolution N 1s spectra are shown in Figure 4b; the Ru n -Ru s /NC and Ru s /NC display similar N peaks, and the characteristic peaks for Ru-N/pyridinic N (398.5 eV) can be detected, [44] which show 0.2 eV higher binding energy than that in Ru n /NC, thus demonstrating that Ru n /NC consists of bare pyridinic N (398.3 eV) and scarcely any Ru-N x species. [45,46] X-ray absorption near edge structure (XANES) spectra of Ru n -Ru s /NC at the Ru K-edge show an average valence between Ru 0 and Ru 4+ (Figure 4c). The integration of XANES spectra quantitatively confirms that the valence state of Ru species in Ru n -Ru s /NC is +1.88 (Figure 4d).…”

Section: Resultsmentioning

confidence: 99%

“…The high‐resolution N 1 s spectra are shown in Figure 4b; the Ru n ‐Ru s /NC and Ru s /NC display similar N peaks, and the characteristic peaks for Ru‐N/pyridinic N (398.5 eV) can be detected, [ 44 ] which show 0.2 eV higher binding energy than that in Ru n /NC, thus demonstrating that Ru n /NC consists of bare pyridinic N (398.3 eV) and scarcely any Ru‐N x species. [ 45,46 ]…”

Section: Resultsmentioning

confidence: 99%

Electronic Structure‐Dependent Water‐Dissociation Pathways of Ruthenium‐Based Catalysts in Alkaline H₂‐Evolution

Yang

Zhao

et al. 2023

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current conditions of electrocatalytic water splitting mainly include acidic and basic media. [5][6][7][8] When considering the huge difficulty in producing affordable acidic oxygen evolution electrodes in water splitting, the electrocatalytic water splitting in alkaline environments has become a meaningful strategy to produce H 2 on a large scale, [9][10][11][12][13] while the commercial alkaline hydrogen evolution reaction (HER) catalyst still relies on the metallic platinum (Pt), which confronts with slow water-dissociation kinetics, poor durability, and high costs. [5,[14][15][16] Highly active and cost-effective HER electrocatalysts are urgently needed for practical water splitting in alkaline conditions, especially alkaline seawater splitting. [17][18][19][20] Among the various transition metal-based hydrogenevolving materials, [21,22] recent studies have disclosed that Ru-based materials can serve as promising alkaline HER electrocatalysts due to their platinum-like electronic structures and relatively low cost (≈1/3 the price of Pt). [23][24][25] Regarding the pursuit of ultrahigh atomic efficiency of Ru metals, substantial efforts have been devoted to synthesizing single-atom Ru catalysts. [26,27] Although single-atom catalytic sites can facilely control the Ru coordination microenvironments and, in principle, obtain 100% atom utilization, these cationic states of single-atom Ru centers can hardly satisfy the alkaline HER electrocatalysis. [28] To increase Ruthenium (Ru)-based catalysts have displayed compelling hydrogen evolution activities, which hold the promising potential to substitute platinum in alkaline H 2 -evolution. In the challenging alkaline electrolytes, the water-dissociation process involves multistep reactions, while the profound origin and intrinsic factors of diverse Ru species on water-dissociation pathways and reaction principles remain ambiguous. Here the fundamental origin of water-dissociation pathways of Ru-based catalysts in alkaline media to be from their unique electronic structures in complex coordination environments are disclosed. These theoretical results validate that the modulated electronic structures with delocalization-localization coexistence at their boundaries between the Ru nanocluster and single-atom site have a profound influence on water-dissociation pathways, which push H 2 O* migration and binding orientation during the splitting process, thus enhancing the dissociation kinetics. By creating Ru catalysts with well-defined nanocluster, single-atom site, and also complex site, the electrocatalytic data shows that both the nanocluster and single-atom play essential roles in water-dissociation, while the complex site possesses synergistically enhanced roles in alkaline electrolytes. This study discloses a new electronic structure-dependent water-dissociation pathway and reaction principle in Ru-based catalysts, thus offering new inspiration to design efficient and durable catalysts for the practical production of H 2 in alkaline electrolytes.

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“…[ 17,18,35,61 ] It is reported that metallo‐enzyme can catalyze H 2 O 2 to generate •OH via oxidation reaction in situ, thereby destroying the biofilm by cleaving the structure of eDNA. [ 19,20 ] However, the half‐life period of ROS molecules are very short (possibly on the nanosecond), and were easily decomposed into other oxidizing species. Therefore, GOx loaded in nanozymes to catalyze non‐toxic glucose to achieve cascade catalysis may be an effective strategy to increase ROS.…”

Section: Introductionmentioning

confidence: 99%

Macrophage Polarization Induced by Bacteria‐Responsive Antibiotic‐Loaded Nanozymes for Multidrug Resistance‐Bacterial Infections Management

Zhu

Guo

Yang

et al. 2023

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Inherited bacterial resistance and biofilm‐induced local immune inactivation are important factors in the failure of antibiotics to fight against bacterial infections. Herein, antibiotic‐loaded mesoporous nanozymes (HA@MRuO2‐Cip/GOx) are fabricated for overcoming bacterial resistance, and activating the local immunosuppression in biofilm microenvironment (BME). HA@MRuO2‐Cip/GOx are prepared by physical adsorption between ciprofloxacin (Cip) or glucose oxidase (GOx) and MRuO2 NPs, and modified with hyaluronic acid (HA). In vitro, HA@MRuO2‐Cip/GOx cleaves extracellular DNA (eDNA) to disrupt biofilm, thereby enhancing Cip kill planktonic bacteria. Furthermore, HA@MRuO2‐Cip/GOx can induce polarization and enhance phagocytosis of a macrophage‐derived cell line. More importantly, in vivo therapeutic performance confirms that HA@MRuO2‐Cip/GOx can trigger macrophage‐related immunity, and effectively alleviate MRSA‐bacterial lung infections. Accordingly, nanocatalytic therapy combined with targeted delivery of antibiotics could enhance the treatment of bacterial infections.

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A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers (Adv. Mater. 16/2022)

Cited by 18 publications

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Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Electronic Structure‐Dependent Water‐Dissociation Pathways of Ruthenium‐Based Catalysts in Alkaline H₂‐Evolution

Macrophage Polarization Induced by Bacteria‐Responsive Antibiotic‐Loaded Nanozymes for Multidrug Resistance‐Bacterial Infections Management

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A Library of ROS‐Catalytic Metalloenzyme Mimics with Atomic Metal Centers (Adv. Mater. 16/2022)

Cited by 18 publications

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Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Catalase‐Mimetic Artificial Biocatalysts with Ru Catalytic Centers for ROS Elimination and Stem‐Cell Protection

Electronic Structure‐Dependent Water‐Dissociation Pathways of Ruthenium‐Based Catalysts in Alkaline H2‐Evolution

Macrophage Polarization Induced by Bacteria‐Responsive Antibiotic‐Loaded Nanozymes for Multidrug Resistance‐Bacterial Infections Management

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Electronic Structure‐Dependent Water‐Dissociation Pathways of Ruthenium‐Based Catalysts in Alkaline H₂‐Evolution