Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments
Abstract High-entropy alloys (HEAs) present a vast compositional space for fine-tuning electrocatalytic activities, leveraging millions of distinct active sites on the surface. However, the intricate local chemical environment poses challenges to the rational and efficient design of HEA electrocatal...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56421-9 |
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| author | Guolin Cao Sha Yang Ji-Chang Ren Wei Liu |
| author_facet | Guolin Cao Sha Yang Ji-Chang Ren Wei Liu |
| author_sort | Guolin Cao |
| collection | DOAJ |
| description | Abstract High-entropy alloys (HEAs) present a vast compositional space for fine-tuning electrocatalytic activities, leveraging millions of distinct active sites on the surface. However, the intricate local chemical environment poses challenges to the rational and efficient design of HEA electrocatalysts with high reactivity. Here, focusing on noble-metal HEAs for oxygen reduction reactions, we propose a straightforward yet effective descriptor for quantitively determining the local reactivities of HEAs. This descriptor is based on a linear combination of the intrinsic d-band filling of the active center and the neighborhood electronegativity. Our model offers an accurate and robust description of the binding strengths of intermediates with different adsorption configurations on HEAs, supported by external density functional theory calculations. Importantly, the local environmental electronegativity of the HEA surface is strongly related to the d-band profile of the center atom(s) embedded within. Finally, we establish a library of activity maps for HEAs encompassing nine noble-metal elements, suggesting that Pd-rich and Ir-rich alloys, such as Pd–Ag, Ir–Pt, Ir–Au compositions, hold promise as potential candidates for optimal electrocatalysts. |
| format | Article |
| id | doaj-art-7e44e3262d1f472ba736c3bbfd472b28 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-7e44e3262d1f472ba736c3bbfd472b282025-02-02T12:31:14ZengNature PortfolioNature Communications2041-17232025-02-0116111110.1038/s41467-025-56421-9Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environmentsGuolin Cao0Sha Yang1Ji-Chang Ren2Wei Liu3Nano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing University of Science and TechnologyNano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing University of Science and TechnologyNano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing University of Science and TechnologyNano and Heterogeneous Materials Center, School of Materials Science and Engineering, Nanjing University of Science and TechnologyAbstract High-entropy alloys (HEAs) present a vast compositional space for fine-tuning electrocatalytic activities, leveraging millions of distinct active sites on the surface. However, the intricate local chemical environment poses challenges to the rational and efficient design of HEA electrocatalysts with high reactivity. Here, focusing on noble-metal HEAs for oxygen reduction reactions, we propose a straightforward yet effective descriptor for quantitively determining the local reactivities of HEAs. This descriptor is based on a linear combination of the intrinsic d-band filling of the active center and the neighborhood electronegativity. Our model offers an accurate and robust description of the binding strengths of intermediates with different adsorption configurations on HEAs, supported by external density functional theory calculations. Importantly, the local environmental electronegativity of the HEA surface is strongly related to the d-band profile of the center atom(s) embedded within. Finally, we establish a library of activity maps for HEAs encompassing nine noble-metal elements, suggesting that Pd-rich and Ir-rich alloys, such as Pd–Ag, Ir–Pt, Ir–Au compositions, hold promise as potential candidates for optimal electrocatalysts.https://doi.org/10.1038/s41467-025-56421-9 |
| spellingShingle | Guolin Cao Sha Yang Ji-Chang Ren Wei Liu Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments Nature Communications |
| title | Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments |
| title_full | Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments |
| title_fullStr | Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments |
| title_full_unstemmed | Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments |
| title_short | Electronic descriptors for designing high-entropy alloy electrocatalysts by leveraging local chemical environments |
| title_sort | electronic descriptors for designing high entropy alloy electrocatalysts by leveraging local chemical environments |
| url | https://doi.org/10.1038/s41467-025-56421-9 |
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