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| Main Authors: | , , , , , , , , |
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| Format: | Preprint |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2411.01727 |
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| _version_ | 1866914009885704192 |
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| author | Jeong, Chaehwa Lee, Juhyeok Jo, Hyesung Lee, KwangHo Lee, SangJae Ophus, Colin Ercius, Peter Cho, EunAe Yang, Yongsoo |
| author_facet | Jeong, Chaehwa Lee, Juhyeok Jo, Hyesung Lee, KwangHo Lee, SangJae Ophus, Colin Ercius, Peter Cho, EunAe Yang, Yongsoo |
| contents | Pt-based electrocatalysts are the primary choice for fuel cells due to their superior oxygen reduction reaction (ORR) activity. To enhance ORR performance and durability, extensive studies have investigated transition metal alloying, doping, and shape control to optimize the three key governing factors for ORR: geometry, local chemistry, and strain of their surface and subsurface. However, systematic optimization remains incomplete, as it requires an atomic-scale understanding of these factors and their dynamics over potential cycling, as well as their relationship to ORR activity. Here, we implement neural network-assisted atomic electron tomography to measure the 3D atomic structural dynamics and their effects on the functional degradation of PtNi alloy catalysts. Our results reveal that PtNi catalysts undergo shape changes, surface alloying, and strain relaxation during cycling, which can be effectively mitigated by Ga doping. By combining geometry, local chemistry, and strain analysis, we calculated the changes in ORR activity over thousands of cycles and observed that Ga doping leads to higher initial activity and greater stability. These findings offer a pathway to understanding 3D atomic structural dynamics and their relation to ORR activity during cycling, paving the way for the systematic design of durable, high-efficiency nanocatalysts. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2411_01727 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Atomic-scale 3D structural dynamics and functional degradation of Pt alloy nanocatalysts during the oxygen reduction reaction Jeong, Chaehwa Lee, Juhyeok Jo, Hyesung Lee, KwangHo Lee, SangJae Ophus, Colin Ercius, Peter Cho, EunAe Yang, Yongsoo Materials Science Applied Physics Pt-based electrocatalysts are the primary choice for fuel cells due to their superior oxygen reduction reaction (ORR) activity. To enhance ORR performance and durability, extensive studies have investigated transition metal alloying, doping, and shape control to optimize the three key governing factors for ORR: geometry, local chemistry, and strain of their surface and subsurface. However, systematic optimization remains incomplete, as it requires an atomic-scale understanding of these factors and their dynamics over potential cycling, as well as their relationship to ORR activity. Here, we implement neural network-assisted atomic electron tomography to measure the 3D atomic structural dynamics and their effects on the functional degradation of PtNi alloy catalysts. Our results reveal that PtNi catalysts undergo shape changes, surface alloying, and strain relaxation during cycling, which can be effectively mitigated by Ga doping. By combining geometry, local chemistry, and strain analysis, we calculated the changes in ORR activity over thousands of cycles and observed that Ga doping leads to higher initial activity and greater stability. These findings offer a pathway to understanding 3D atomic structural dynamics and their relation to ORR activity during cycling, paving the way for the systematic design of durable, high-efficiency nanocatalysts. |
| title | Atomic-scale 3D structural dynamics and functional degradation of Pt alloy nanocatalysts during the oxygen reduction reaction |
| topic | Materials Science Applied Physics |
| url | https://arxiv.org/abs/2411.01727 |