An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites
Chemical looping air separation (CLAS) is a promising process intensification technology for extracting oxygen from air for oxygen enrichment in process streams. Co-doped strontium ferrites (SrFe1-xCoxO3-δ) have been found to have outstanding activities for CLAS processes. In this study, we explore...
| Main Authors: | , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Online Access: | https://hdl.handle.net/10356/179376 |
| _version_ | 1811687772766863360 |
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| author | Fan, Qianwenhao Li, Haiyan Saqline, Syed Donat, Felix Tan, Mingwu Tao, Longgang Müller, Christoph R. Xu, Jason Zhichuan Liu, Wen |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Fan, Qianwenhao Li, Haiyan Saqline, Syed Donat, Felix Tan, Mingwu Tao, Longgang Müller, Christoph R. Xu, Jason Zhichuan Liu, Wen |
| author_sort | Fan, Qianwenhao |
| collection | NTU |
| description | Chemical looping air separation (CLAS) is a promising process intensification technology for extracting oxygen from air for oxygen enrichment in process streams. Co-doped strontium ferrites (SrFe1-xCoxO3-δ) have been found to have outstanding activities for CLAS processes. In this study, we explore the underlying factors driving the enhancement in oxygen uptake and release performance of perovskite structured SrFe1-xCoxO3-δ oxygen carriers for CLAS. Phase-pure perovskites, with B site substituted by up to 75 mol% Co, were prepared by a sol-gel method and systematically investigated through a wide range of well controlled experimental and computational approaches. While all SrFe1-xCoxO3-δ oxygen carriers showed excellent cyclic stability and structural reversibility over CLAS cycles, increased B site occupancy by Co resulted in monotonic decrease in onset temperature for oxygen release and increase in oxygen carrying capacity. These experimental trends can be fundamentally explained by an increase in the structural tolerance factor, an elevation in transition metal d-band, as well as an increased degree of hybridization between the metal d-band and the O p band. Therefore, these ab initio structural and electronic descriptors are useful design rationales for the hypothesis-driven synthesis of high-performing oxygen carriers for CLAS. |
| first_indexed | 2024-10-01T05:21:38Z |
| format | Journal Article |
| id | ntu-10356/179376 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:21:38Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1793762024-08-02T15:31:40Z An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites Fan, Qianwenhao Li, Haiyan Saqline, Syed Donat, Felix Tan, Mingwu Tao, Longgang Müller, Christoph R. Xu, Jason Zhichuan Liu, Wen School of Chemistry, Chemical Engineering and Biotechnology School of Materials Science and Engineering Cambridge Centre for Advanced Research and Education in Singapore Nanyang Environment and Water Research Institute Chemistry Air separation Chemical looping Chemical looping air separation (CLAS) is a promising process intensification technology for extracting oxygen from air for oxygen enrichment in process streams. Co-doped strontium ferrites (SrFe1-xCoxO3-δ) have been found to have outstanding activities for CLAS processes. In this study, we explore the underlying factors driving the enhancement in oxygen uptake and release performance of perovskite structured SrFe1-xCoxO3-δ oxygen carriers for CLAS. Phase-pure perovskites, with B site substituted by up to 75 mol% Co, were prepared by a sol-gel method and systematically investigated through a wide range of well controlled experimental and computational approaches. While all SrFe1-xCoxO3-δ oxygen carriers showed excellent cyclic stability and structural reversibility over CLAS cycles, increased B site occupancy by Co resulted in monotonic decrease in onset temperature for oxygen release and increase in oxygen carrying capacity. These experimental trends can be fundamentally explained by an increase in the structural tolerance factor, an elevation in transition metal d-band, as well as an increased degree of hybridization between the metal d-band and the O p band. Therefore, these ab initio structural and electronic descriptors are useful design rationales for the hypothesis-driven synthesis of high-performing oxygen carriers for CLAS. Ministry of Education (MOE) National Research Foundation (NRF) Published version The authors would like to thank the financial support by Ministry of Education Singapore’s Academic Research Fund Tier 1 (RT03/19 and RG112/18) and the National Research Foundation (NRF), Prime Minister’s Office, Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. 2024-07-29T02:32:27Z 2024-07-29T02:32:27Z 2024 Journal Article Fan, Q., Li, H., Saqline, S., Donat, F., Tan, M., Tao, L., Müller, C. R., Xu, J. Z. & Liu, W. (2024). An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites. Physical Chemistry Chemical Physics. https://dx.doi.org/10.1039/d4cp02152e 1463-9076 https://hdl.handle.net/10356/179376 10.1039/d4cp02152e 39034776 2-s2.0-85199302845 en RT03/19 RG112/18 CREATE Physical Chemistry Chemical Physics 10.21979/N9/OGIWAS © The Author(s). This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. application/pdf |
| spellingShingle | Chemistry Air separation Chemical looping Fan, Qianwenhao Li, Haiyan Saqline, Syed Donat, Felix Tan, Mingwu Tao, Longgang Müller, Christoph R. Xu, Jason Zhichuan Liu, Wen An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title | An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title_full | An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title_fullStr | An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title_full_unstemmed | An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title_short | An investigation of the structural and electronic origins of enhanced chemical looping air separation performance of B-site substituted SrFe1-xCoxO3-δ perovskites |
| title_sort | investigation of the structural and electronic origins of enhanced chemical looping air separation performance of b site substituted srfe1 xcoxo3 δ perovskites |
| topic | Chemistry Air separation Chemical looping |
| url | https://hdl.handle.net/10356/179376 |
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