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Metal-ligand dual-site single-atom nanozyme mimicking urate oxidase with high substrates specificity.

التفاصيل البيبلوغرافية
العنوان: Metal-ligand dual-site single-atom nanozyme mimicking urate oxidase with high substrates specificity.
المؤلفون: Wang K; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Hong Q; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Zhu C; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Xu Y; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Li W; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Wang Y; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Chen W; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Gu X; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Chen X; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Fang Y; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Shen Y; Medical School, Southeast University, Nanjing, 210009, China. Yanfei.Shen@seu.edu.cn., Liu S; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China., Zhang Y; Jiangsu Engineering Research Center for Carbon-Rich Materials and Devices, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Nanjing, 211189, China. Yuanjian.Zhang@seu.edu.cn.; Department of Oncology, Zhongda Hospital, Southeast University, Nanjing, 210009, China. Yuanjian.Zhang@seu.edu.cn.
المصدر: Nature communications [Nat Commun] 2024 Jul 08; Vol. 15 (1), pp. 5705. Date of Electronic Publication: 2024 Jul 08.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: Nature Pub. Group Country of Publication: England NLM ID: 101528555 Publication Model: Electronic Cited Medium: Internet ISSN: 2041-1723 (Electronic) Linking ISSN: 20411723 NLM ISO Abbreviation: Nat Commun Subsets: MEDLINE
أسماء مطبوعة: Original Publication: [London] : Nature Pub. Group
مواضيع طبية MeSH: Urate Oxidase*/chemistry , Urate Oxidase*/metabolism , Uric Acid*/chemistry , Uric Acid*/metabolism , Uric Acid*/urine , Oxidation-Reduction*, Substrate Specificity ; Ligands ; Humans ; Nickel/chemistry ; Nickel/metabolism ; Binding Sites ; Catalytic Domain ; Catalysis ; Models, Molecular ; X-Ray Absorption Spectroscopy
مستخلص: In nature, coenzyme-independent oxidases have evolved in selective catalysis using isolated substrate-binding pockets. Single-atom nanozymes (SAzymes), an emerging type of non-protein artificial enzymes, are promising to simulate enzyme active centers, but owing to the lack of recognition sites, realizing substrate specificity is a formidable task. Here we report a metal-ligand dual-site SAzyme (Ni-DAB) that exhibited selectivity in uric acid (UA) oxidation. Ni-DAB mimics the dual-site catalytic mechanism of urate oxidase, in which the Ni metal center and the C atom in the ligand serve as the specific UA and O 2 binding sites, respectively, characterized by synchrotron soft X-ray absorption spectroscopy, in situ near ambient pressure X-ray photoelectron spectroscopy, and isotope labeling. The theoretical calculations reveal the high catalytic specificity is derived from not only the delicate interaction between UA and the Ni center but also the complementary oxygen reduction at the beta C site in the ligand. As a potential application, a Ni-DAB-based biofuel cell using human urine is constructed. This work unlocks an approach of enzyme-like isolated dual sites in boosting the selectivity of non-protein artificial enzymes.
(© 2024. The Author(s).)
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معلومات مُعتمدة: 22174014 National Natural Science Foundation of China (National Science Foundation of China); 22074015 National Natural Science Foundation of China (National Science Foundation of China)
المشرفين على المادة: EC 1.7.3.3 (Urate Oxidase)
268B43MJ25 (Uric Acid)
0 (Ligands)
7OV03QG267 (Nickel)
تواريخ الأحداث: Date Created: 20240708 Date Completed: 20240708 Latest Revision: 20240802
رمز التحديث: 20240802
مُعرف محوري في PubMed: PMC11231224
DOI: 10.1038/s41467-024-50123-4
PMID: 38977710
قاعدة البيانات: MEDLINE
الوصف
تدمد:2041-1723
DOI:10.1038/s41467-024-50123-4