Cargando…
Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation
The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied sta...
Autores principales: | , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10533845/ https://www.ncbi.nlm.nih.gov/pubmed/37758731 http://dx.doi.org/10.1038/s41467-023-41706-8 |
_version_ | 1785112262139183104 |
---|---|
author | Wang, Fangqing Zou, Peichao Zhang, Yangyang Pan, Wenli Li, Ying Liang, Limin Chen, Cong Liu, Hui Zheng, Shijian |
author_facet | Wang, Fangqing Zou, Peichao Zhang, Yangyang Pan, Wenli Li, Ying Liang, Limin Chen, Cong Liu, Hui Zheng, Shijian |
author_sort | Wang, Fangqing |
collection | PubMed |
description | The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (Au(SA)-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm(−2) and high mass activity of 732.925 A g(−1) at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm(−2). Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity. |
format | Online Article Text |
id | pubmed-10533845 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-105338452023-09-29 Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation Wang, Fangqing Zou, Peichao Zhang, Yangyang Pan, Wenli Li, Ying Liang, Limin Chen, Cong Liu, Hui Zheng, Shijian Nat Commun Article The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (Au(SA)-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm(−2) and high mass activity of 732.925 A g(−1) at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm(−2). Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity. Nature Publishing Group UK 2023-09-27 /pmc/articles/PMC10533845/ /pubmed/37758731 http://dx.doi.org/10.1038/s41467-023-41706-8 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Wang, Fangqing Zou, Peichao Zhang, Yangyang Pan, Wenli Li, Ying Liang, Limin Chen, Cong Liu, Hui Zheng, Shijian Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title | Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title_full | Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title_fullStr | Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title_full_unstemmed | Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title_short | Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation |
title_sort | activating lattice oxygen in high-entropy ldh for robust and durable water oxidation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10533845/ https://www.ncbi.nlm.nih.gov/pubmed/37758731 http://dx.doi.org/10.1038/s41467-023-41706-8 |
work_keys_str_mv | AT wangfangqing activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT zoupeichao activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT zhangyangyang activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT panwenli activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT liying activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT lianglimin activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT chencong activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT liuhui activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation AT zhengshijian activatinglatticeoxygeninhighentropyldhforrobustanddurablewateroxidation |