Using the High-Entropy Approach to Obtain Multimetal Oxide Nanozymes: Library Synthesis, In Silico Structure–Activity, and Immunoassay Performance
High-entropy nanomaterials exhibit exceptional mechanical, physical, and chemical properties, finding applications in many industries. Peroxidases are metalloenzymes that accelerate the decomposition of hydrogen peroxide. This study uses the high-entropy approach to generate multimetal oxide-based n...
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| Veröffentlicht in: | ACS nano 2024-07, Vol.18 (29), p.19024-19037 |
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| creator | Phan-Xuan, Thuong Schweidler, Simon Hirte, Steffen Schüller, Moritz Lin, Ling Khandelwal, Anurag Wang, Kai Schützke, Jan Reischl, Markus Kübel, Christian Hahn, Horst Bello, Gianluca Kirchmair, Johannes Aghassi-Hagmann, Jasmin Brezesinski, Torsten Breitung, Ben Dailey, Lea Ann |
| description | High-entropy nanomaterials exhibit exceptional mechanical, physical, and chemical properties, finding applications in many industries. Peroxidases are metalloenzymes that accelerate the decomposition of hydrogen peroxide. This study uses the high-entropy approach to generate multimetal oxide-based nanozymes with peroxidase-like activity and explores their application as sensors in ex vivo bioassays. A library of 81 materials was produced using a coprecipitation method for rapid synthesis of up to 100 variants in a single plate. The A and B sites of the magnetite structure, (AA‘)(BB’B‘‘)2O4, were substituted with up to six different cations (Cu/Fe/Zn/Mg/Mn/Cr). Increasing the compositional complexity improved the catalytic performance; however, substitutions of single elements also caused drastic reductions in the peroxidase-like activity. A generalized linear model was developed describing the relationship between material composition and catalytic activity. Binary interactions between elements that acted synergistically or antagonistically were identified, and a single parameter, the mean interaction effect, was observed to correlate highly with catalytic activity, providing a valuable tool for the design of high-entropy-inspired nanozymes. |
| doi_str_mv | 10.1021/acsnano.4c03053 |
| format | Article |
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Peroxidases are metalloenzymes that accelerate the decomposition of hydrogen peroxide. This study uses the high-entropy approach to generate multimetal oxide-based nanozymes with peroxidase-like activity and explores their application as sensors in ex vivo bioassays. A library of 81 materials was produced using a coprecipitation method for rapid synthesis of up to 100 variants in a single plate. The A and B sites of the magnetite structure, (AA‘)(BB’B‘‘)2O4, were substituted with up to six different cations (Cu/Fe/Zn/Mg/Mn/Cr). Increasing the compositional complexity improved the catalytic performance; however, substitutions of single elements also caused drastic reductions in the peroxidase-like activity. A generalized linear model was developed describing the relationship between material composition and catalytic activity. Binary interactions between elements that acted synergistically or antagonistically were identified, and a single parameter, the mean interaction effect, was observed to correlate highly with catalytic activity, providing a valuable tool for the design of high-entropy-inspired nanozymes.</description><identifier>ISSN: 1936-0851</identifier><identifier>ISSN: 1936-086X</identifier><identifier>EISSN: 1936-086X</identifier><identifier>DOI: 10.1021/acsnano.4c03053</identifier><identifier>PMID: 38985736</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Catalysis ; Computer Simulation ; Entropy ; Hydrogen Peroxide - chemistry ; Immunoassay - methods ; Nanostructures - chemistry ; Oxides - chemistry ; Structure-Activity Relationship</subject><ispartof>ACS nano, 2024-07, Vol.18 (29), p.19024-19037</ispartof><rights>2024 The Authors. 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| subjects | Catalysis Computer Simulation Entropy Hydrogen Peroxide - chemistry Immunoassay - methods Nanostructures - chemistry Oxides - chemistry Structure-Activity Relationship |
| title | Using the High-Entropy Approach to Obtain Multimetal Oxide Nanozymes: Library Synthesis, In Silico Structure–Activity, and Immunoassay Performance |
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