D-band center coordination modulated enzyme-like activity in Fe-Cu dual-metal single-atom nanozymes
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Xiao-Dong Zhang1,2(
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After explorations in a diversity of single-atom nanozymes (SAzymes), developing dual-centered SAzymes becomes a promising approach for superior catalytic performance. But confusing mechanisms including atomic coordination, spatial configuration, and metal–metal atom interaction hinder the development and design of SAzymes. Herein, a dual-centered Fe-Cu-Nx SAzyme exhibits excellent peroxidase (POD)- and catalase (CAT)-like activities with d-band center (εd) coordination of Fe and Cu in multiple reaction stages, which plays a critical role in the adsorption of H2O2 molecule and H2O and O2 release. Therefore, the d-band center coordination, which can be represented by εd(Fe)–εd(Cu) shifts, leads to the competition between one-side and bilateral adsorption, which determines the favorable reaction path with lower energy barriers. Based on experimental statistics, simulated formation energies, and reaction barriers, 3 configurations, Fe-Cu-N6-I, Fe-Cu-N8-II, and Fe-Cu-N8-III, are modeled and validated. Impressively, configuration-dependent catalytic selectivity and the competition between one-side and bilateral adsorption can be unveiled by d-band center coordination paradigm analysis. Theoretical simulations suggest that the unsymmetrical charge distribution over the three Fe-Cu configurations could tune the adsorption strength compared with the counterparts FeN4 and CuN4. The present work provides a potential route for optimizing enzyme-like catalysis by designing the dual- or even triple-metal SAzymes, which demonstrates the large space to modulate the metal atomic configuration and interaction.
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D-band center coordination modulated enzyme-like activity in Fe-Cu dual-metal single-atom nanozymes
), Xiao-Dong Zhang1,2(
)
Abstract
After explorations in a diversity of single-atom nanozymes (SAzymes), developing dual-centered SAzymes becomes a promising approach for superior catalytic performance. But confusing mechanisms including atomic coordination, spatial configuration, and metal–metal atom interaction hinder the development and design of SAzymes. Herein, a dual-centered Fe-Cu-Nx SAzyme exhibits excellent peroxidase (POD)- and catalase (CAT)-like activities with d-band center (εd) coordination of Fe and Cu in multiple reaction stages, which plays a critical role in the adsorption of H2O2 molecule and H2O and O2 release. Therefore, the d-band center coordination, which can be represented by εd(Fe)–εd(Cu) shifts, leads to the competition between one-side and bilateral adsorption, which determines the favorable reaction path with lower energy barriers. Based on experimental statistics, simulated formation energies, and reaction barriers, 3 configurations, Fe-Cu-N6-I, Fe-Cu-N8-II, and Fe-Cu-N8-III, are modeled and validated. Impressively, configuration-dependent catalytic selectivity and the competition between one-side and bilateral adsorption can be unveiled by d-band center coordination paradigm analysis. Theoretical simulations suggest that the unsymmetrical charge distribution over the three Fe-Cu configurations could tune the adsorption strength compared with the counterparts FeN4 and CuN4. The present work provides a potential route for optimizing enzyme-like catalysis by designing the dual- or even triple-metal SAzymes, which demonstrates the large space to modulate the metal atomic configuration and interaction.
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Acknowledgements
This work was financially supported by the National Key Research and Development Program of China (Nos. 2021YFF1200700 and 2021YFF1200701), the National Natural Science Foundation of China (Nos. 91859101, 81971744, U1932107, 82001952, 11804248, 82302361, and 82302381), Outstanding Youth Funds of Tianjin (No. 2021FJ-0009), STI 2030-Major Projects (No. 2022ZD0210200)， National Natural Science Foundation of Tianjin (Nos. 19JCZDJC34000, 20JCYBJC00940, 21JCYBJC00550, 21JCZDJC00620, and 21JCYBJC00490), the Key Projects of Tianjin Natural Fund (No. 21JCZDJC00490), the Innovation Foundation of Tianjin University, China Postdoctoral Science Foundation (No. 2023M732601), and CAS Interdisciplinary Innovation Team (No. JCTD-2020-08).
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