Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability

Ni–Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction (OER) in water electrolysis. However, understanding and mastering the synergy of Ni and Fe remain challenging. Herein, we report that the synergy between Ni and Fe can be tailored...

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Main Authors: Zhang, H., Guan, D., Gu, Y., Xu, Hengyue, Wang, C., Shao, Zongping, Guo, Y.
Format: Journal Article
Published: 2024
Online Access:http://purl.org/au-research/grants/arc/DP200103332
http://hdl.handle.net/20.500.11937/94760
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author Zhang, H.
Guan, D.
Gu, Y.
Xu, Hengyue
Wang, C.
Shao, Zongping
Guo, Y.
author_facet Zhang, H.
Guan, D.
Gu, Y.
Xu, Hengyue
Wang, C.
Shao, Zongping
Guo, Y.
author_sort Zhang, H.
building Curtin Institutional Repository
collection Online Access
description Ni–Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction (OER) in water electrolysis. However, understanding and mastering the synergy of Ni and Fe remain challenging. Herein, we report that the synergy between Ni and Fe can be tailored by crystal dimensionality of Ni, Fe-contained Ruddlesden–Popper (RP)-type perovskites (La0.125Sr0.875)n+1(Ni0.25Fe0.75)nO3n+1 (n = 1, 2, 3), where the material with n = 3 shows the best OER performance in alkaline media. Soft X-ray absorption spectroscopy spectra before and after OER reveal that the material with n = 3 shows enhanced Ni/Fe–O covalency to boost the electron transfer as compared to those with n = 1 and n = 2. Further experimental investigations demonstrate that the Fe ion is the active site and the Ni ion is the stable site in this system, where such unique synergy reaches the optimum at n = 3. Besides, as n increases, the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions (especially Sr2+) into the electrolyte is suppressed, which induces a decrease in the leaching of active Fe ions, ultimately leading to enhanced stability. This work provides a new avenue for rational catalyst design through the dimensional strategy.
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spelling curtin-20.500.11937-947602024-05-22T03:53:27Z Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability Zhang, H. Guan, D. Gu, Y. Xu, Hengyue Wang, C. Shao, Zongping Guo, Y. Ni–Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction (OER) in water electrolysis. However, understanding and mastering the synergy of Ni and Fe remain challenging. Herein, we report that the synergy between Ni and Fe can be tailored by crystal dimensionality of Ni, Fe-contained Ruddlesden–Popper (RP)-type perovskites (La0.125Sr0.875)n+1(Ni0.25Fe0.75)nO3n+1 (n = 1, 2, 3), where the material with n = 3 shows the best OER performance in alkaline media. Soft X-ray absorption spectroscopy spectra before and after OER reveal that the material with n = 3 shows enhanced Ni/Fe–O covalency to boost the electron transfer as compared to those with n = 1 and n = 2. Further experimental investigations demonstrate that the Fe ion is the active site and the Ni ion is the stable site in this system, where such unique synergy reaches the optimum at n = 3. Besides, as n increases, the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions (especially Sr2+) into the electrolyte is suppressed, which induces a decrease in the leaching of active Fe ions, ultimately leading to enhanced stability. This work provides a new avenue for rational catalyst design through the dimensional strategy. 2024 Journal Article http://hdl.handle.net/20.500.11937/94760 10.1002/cey2.465 http://purl.org/au-research/grants/arc/DP200103332 http://purl.org/au-research/grants/arc/DP200103315 http://creativecommons.org/licenses/by/4.0/ fulltext
spellingShingle Zhang, H.
Guan, D.
Gu, Y.
Xu, Hengyue
Wang, C.
Shao, Zongping
Guo, Y.
Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title_full Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title_fullStr Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title_full_unstemmed Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title_short Tuning synergy between nickel and iron in Ruddlesden–Popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
title_sort tuning synergy between nickel and iron in ruddlesden–popper perovskites through controllable crystal dimensionalities towards enhanced oxygen-evolving activity and stability
url http://purl.org/au-research/grants/arc/DP200103332
http://purl.org/au-research/grants/arc/DP200103332
http://hdl.handle.net/20.500.11937/94760