Entropy-driven difference in interfacial water reactivity between slab and nanodroplet
Abstract Interfacial water activity plays a critical role in governing chemical reactivity and catalytic efficiency, yet a quantitative understanding of how hydrogen-bond (H-bond) network structure influences this reactivity remains limited. Herein, we employ ab initio molecular metadynamics simulat...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-60298-z |
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| author | Shiwei Chen Jiabao Zhu Jifan Li Pan Guo Jinrong Yang Xiao He |
| author_facet | Shiwei Chen Jiabao Zhu Jifan Li Pan Guo Jinrong Yang Xiao He |
| author_sort | Shiwei Chen |
| collection | DOAJ |
| description | Abstract Interfacial water activity plays a critical role in governing chemical reactivity and catalytic efficiency, yet a quantitative understanding of how hydrogen-bond (H-bond) network structure influences this reactivity remains limited. Herein, we employ ab initio molecular metadynamics simulations to delineate the relationship between the H-bond network and the reactivity of interfacial water molecules at the slab and nanodroplet systems. Interfacial water at nanodroplets, characterized by microscopic inhomogeneity, tends to adopt a donor–acceptor dimer configuration, in contrast to the more homogeneous H-bond network at the slab. This disparity in local structure, corroborated by the quantified differences in solvation configurational entropy, results in a reduction of the reaction free energy barrier by 1–2 kcal·mol⁻1 at the slab interface, corresponding to an order-of-magnitude enhancement in reaction rate. These results provide a fresh perspective to understand the interfacial water reactivity and highlight the critical role of H-bond network in optimizing catalytic performance. |
| format | Article |
| id | doaj-art-3eaa67051cf645d7bdfcf0d0676257e8 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-3eaa67051cf645d7bdfcf0d0676257e82025-08-20T03:26:43ZengNature PortfolioNature Communications2041-17232025-06-0116111210.1038/s41467-025-60298-zEntropy-driven difference in interfacial water reactivity between slab and nanodropletShiwei Chen0Jiabao Zhu1Jifan Li2Pan Guo3Jinrong Yang4Xiao He5Shanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan RdShanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan RdShanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan RdDepartment of Physics, Shanghai Key Laboratory of High Temperature Superconductors, International Centre of Quantum and Molecular Structures, Shanghai UniversityShanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan RdShanghai Engineering Research Center of Molecular Therapeutics and New Drug Development, Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, School of Chemistry and Molecular Engineering, East China Normal University, 3663 North Zhongshan RdAbstract Interfacial water activity plays a critical role in governing chemical reactivity and catalytic efficiency, yet a quantitative understanding of how hydrogen-bond (H-bond) network structure influences this reactivity remains limited. Herein, we employ ab initio molecular metadynamics simulations to delineate the relationship between the H-bond network and the reactivity of interfacial water molecules at the slab and nanodroplet systems. Interfacial water at nanodroplets, characterized by microscopic inhomogeneity, tends to adopt a donor–acceptor dimer configuration, in contrast to the more homogeneous H-bond network at the slab. This disparity in local structure, corroborated by the quantified differences in solvation configurational entropy, results in a reduction of the reaction free energy barrier by 1–2 kcal·mol⁻1 at the slab interface, corresponding to an order-of-magnitude enhancement in reaction rate. These results provide a fresh perspective to understand the interfacial water reactivity and highlight the critical role of H-bond network in optimizing catalytic performance.https://doi.org/10.1038/s41467-025-60298-z |
| spellingShingle | Shiwei Chen Jiabao Zhu Jifan Li Pan Guo Jinrong Yang Xiao He Entropy-driven difference in interfacial water reactivity between slab and nanodroplet Nature Communications |
| title | Entropy-driven difference in interfacial water reactivity between slab and nanodroplet |
| title_full | Entropy-driven difference in interfacial water reactivity between slab and nanodroplet |
| title_fullStr | Entropy-driven difference in interfacial water reactivity between slab and nanodroplet |
| title_full_unstemmed | Entropy-driven difference in interfacial water reactivity between slab and nanodroplet |
| title_short | Entropy-driven difference in interfacial water reactivity between slab and nanodroplet |
| title_sort | entropy driven difference in interfacial water reactivity between slab and nanodroplet |
| url | https://doi.org/10.1038/s41467-025-60298-z |
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