A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution
Perovskite oxides are of particular interest for the oxygen evolution reaction (OER) due to their high intrinsic activity. However, low surface area and nonpores in bulk phase generally limit the mass transport and thereby result in unsatisfactory mass activity. Herein, we propose a "molecular-...
| Main Authors: | , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Online Access: | https://hdl.handle.net/10356/153627 |
| _version_ | 1811687022070333440 |
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| author | She, Sixuan Zhu, Yinlong Tahini, Hassan A. Hu, Zhiwei Weng, Shih-Chang Wu, Xinhao Chen, Yubo Guan, Daqin Song, Yufei Dai, Jie Smith, Sean C. Wang, Huanting Zhou, Wei Shao, Zongping |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering She, Sixuan Zhu, Yinlong Tahini, Hassan A. Hu, Zhiwei Weng, Shih-Chang Wu, Xinhao Chen, Yubo Guan, Daqin Song, Yufei Dai, Jie Smith, Sean C. Wang, Huanting Zhou, Wei Shao, Zongping |
| author_sort | She, Sixuan |
| collection | NTU |
| description | Perovskite oxides are of particular interest for the oxygen evolution reaction (OER) due to their high intrinsic activity. However, low surface area and nonpores in bulk phase generally limit the mass transport and thereby result in unsatisfactory mass activity. Herein, we propose a "molecular-level strategy"with the simultaneous modulation of the ordered pores on the oxygen-deficient sites along with sulfur (S) substitution on oxygen sites at the molecular level to boost the mass transport behavior of perovskite electrocatalyst for enhanced mass activity. As a proof of concept, the elaborately designed brownmillerite oxide Sr2Co1.6Fe0.4O4.8S0.2 (S-BM-SCF) shows approximately fourfold mass activity enhancement in 1 M KOH compared with the pristine SrCo0.8Fe0.2O3-δ (SCF) perovskite. Comprehensive experimental results, in combination with theoretical calculations, demonstrate that the intrinsic molecular-level pores in the brownmillerite structure can facilitate reactive hydroxyl ion (OH-) uptake into the oxygen-vacant sites and that S doping further promotes OH- adsorption by electronic structure modulation, thus accelerating mass transport rate. Meanwhile, the S-BM-SCF can significantly weaken the resistance of O2 desorption on the catalyst surface, facilitating the O2 evolution. This work deepens the understanding of how mass transport impacts the kinetics of the OER process and opens up a new avenue to design high-performance catalysts on the molecular level. |
| first_indexed | 2024-10-01T05:09:42Z |
| format | Journal Article |
| id | ntu-10356/153627 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:09:42Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1536272023-07-14T15:46:40Z A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution She, Sixuan Zhu, Yinlong Tahini, Hassan A. Hu, Zhiwei Weng, Shih-Chang Wu, Xinhao Chen, Yubo Guan, Daqin Song, Yufei Dai, Jie Smith, Sean C. Wang, Huanting Zhou, Wei Shao, Zongping School of Materials Science and Engineering Engineering::Materials Electrocatalysts Electronic Structure Perovskite oxides are of particular interest for the oxygen evolution reaction (OER) due to their high intrinsic activity. However, low surface area and nonpores in bulk phase generally limit the mass transport and thereby result in unsatisfactory mass activity. Herein, we propose a "molecular-level strategy"with the simultaneous modulation of the ordered pores on the oxygen-deficient sites along with sulfur (S) substitution on oxygen sites at the molecular level to boost the mass transport behavior of perovskite electrocatalyst for enhanced mass activity. As a proof of concept, the elaborately designed brownmillerite oxide Sr2Co1.6Fe0.4O4.8S0.2 (S-BM-SCF) shows approximately fourfold mass activity enhancement in 1 M KOH compared with the pristine SrCo0.8Fe0.2O3-δ (SCF) perovskite. Comprehensive experimental results, in combination with theoretical calculations, demonstrate that the intrinsic molecular-level pores in the brownmillerite structure can facilitate reactive hydroxyl ion (OH-) uptake into the oxygen-vacant sites and that S doping further promotes OH- adsorption by electronic structure modulation, thus accelerating mass transport rate. Meanwhile, the S-BM-SCF can significantly weaken the resistance of O2 desorption on the catalyst surface, facilitating the O2 evolution. This work deepens the understanding of how mass transport impacts the kinetics of the OER process and opens up a new avenue to design high-performance catalysts on the molecular level. Published version This work was supported by National Natural Science Foundation of China (Grant Nos. 21576135 and 21878158) and Jiangsu Natural Science Foundation for Distinguished Young Scholars (Grant No. BK20170043). Dr. H. A. Tahini acknowledges the resources provided by the National Computational Infrastructure (NCI) facility at the Australian National University through the National Computational Merit Allocation Scheme. Dr. Y. Zhu acknowledges the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005, and Discovery Project No. DP200100500). We acknowledge support from the Max Planck-POSTECH/Hsinchu Center for Complex Phase Materials. 2022-01-07T03:19:00Z 2022-01-07T03:19:00Z 2021 Journal Article She, S., Zhu, Y., Tahini, H. A., Hu, Z., Weng, S., Wu, X., Chen, Y., Guan, D., Song, Y., Dai, J., Smith, S. C., Wang, H., Zhou, W. & Shao, Z. (2021). A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution. Applied Physics Reviews, 8(1), 011407-. https://dx.doi.org/10.1063/5.0033912 1931-9401 https://hdl.handle.net/10356/153627 10.1063/5.0033912 2-s2.0-85102006112 1 8 011407 en Applied Physics Reviews © 2021 Author(s). Published under license by AIP Publishing. application/pdf |
| spellingShingle | Engineering::Materials Electrocatalysts Electronic Structure She, Sixuan Zhu, Yinlong Tahini, Hassan A. Hu, Zhiwei Weng, Shih-Chang Wu, Xinhao Chen, Yubo Guan, Daqin Song, Yufei Dai, Jie Smith, Sean C. Wang, Huanting Zhou, Wei Shao, Zongping A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title | A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title_full | A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title_fullStr | A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title_full_unstemmed | A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title_short | A molecular-level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| title_sort | molecular level strategy to boost the mass transport of perovskite electrocatalyst for enhanced oxygen evolution |
| topic | Engineering::Materials Electrocatalysts Electronic Structure |
| url | https://hdl.handle.net/10356/153627 |
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