Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles
Solar thermochemical CO2-splitting (STCS) is a promising solution for solar energy harvesting and storage. However, practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers, resulting in slow reaction kineti...
| Main Authors: | , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/155655 |
| _version_ | 1811693481367699456 |
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| author | Hu, Yue Wu, Jian Han, Yujia Xu, Weibin Zhang, Li Xia, Xue Huang, Chuande Zhu, Yanyan Tian, Ming Su, Yang Li, Lin Hou, Baolin Lin, Jian Liu, Wen Wang, Xiaodong |
| author2 | School of Chemical and Biomedical Engineering |
| author_facet | School of Chemical and Biomedical Engineering Hu, Yue Wu, Jian Han, Yujia Xu, Weibin Zhang, Li Xia, Xue Huang, Chuande Zhu, Yanyan Tian, Ming Su, Yang Li, Lin Hou, Baolin Lin, Jian Liu, Wen Wang, Xiaodong |
| author_sort | Hu, Yue |
| collection | NTU |
| description | Solar thermochemical CO2-splitting (STCS) is a promising solution for solar energy harvesting and storage. However, practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers, resulting in slow reaction kinetics and limited CO2 conversion. Here, we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS process. The novel material achieved an unprecedented CO production rate of 381 mL g−1 min−1 with 99% CO2 conversion at 850 °C, outperforming state-of-the-art materials. In situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO2 splitting. Preferential oxidation of the FeNi alloy at the interface (as opposed to forming an FeOx passivation shell encapsulating bare metallic iron) and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO2 to CO. Facile regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas (H2/CO = 2, syngas yield > 96%). Overall, the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production, with a theoretical solar-to-fuel efficiency of up to 58%, in the absence of any heat integration. |
| first_indexed | 2024-10-01T06:52:22Z |
| format | Journal Article |
| id | ntu-10356/155655 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:52:22Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1556552023-12-29T06:51:22Z Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles Hu, Yue Wu, Jian Han, Yujia Xu, Weibin Zhang, Li Xia, Xue Huang, Chuande Zhu, Yanyan Tian, Ming Su, Yang Li, Lin Hou, Baolin Lin, Jian Liu, Wen Wang, Xiaodong School of Chemical and Biomedical Engineering Engineering::Chemical engineering CO₂ Splitting Iron‐Nickel Alloy Solar thermochemical CO2-splitting (STCS) is a promising solution for solar energy harvesting and storage. However, practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers, resulting in slow reaction kinetics and limited CO2 conversion. Here, we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS process. The novel material achieved an unprecedented CO production rate of 381 mL g−1 min−1 with 99% CO2 conversion at 850 °C, outperforming state-of-the-art materials. In situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO2 splitting. Preferential oxidation of the FeNi alloy at the interface (as opposed to forming an FeOx passivation shell encapsulating bare metallic iron) and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO2 to CO. Facile regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas (H2/CO = 2, syngas yield > 96%). Overall, the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production, with a theoretical solar-to-fuel efficiency of up to 58%, in the absence of any heat integration. Submitted/Accepted version 2022-03-11T05:27:03Z 2022-03-11T05:27:03Z 2021 Journal Article Hu, Y., Wu, J., Han, Y., Xu, W., Zhang, L., Xia, X., Huang, C., Zhu, Y., Tian, M., Su, Y., Li, L., Hou, B., Lin, J., Liu, W. & Wang, X. (2021). Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles. Chinese Journal of Catalysis, 42(11), 2049-2058. https://dx.doi.org/10.1016/S1872-2067(21)63857-3 1872-2067 https://hdl.handle.net/10356/155655 10.1016/S1872-2067(21)63857-3 2-s2.0-85124659015 11 42 2049 2058 en Chinese Journal of Catalysis © 2021 Dalian Institute of Chemical Physics, Chinese Academy of Sciences. All rights reserved. This paper was published by Elsevier B.V. in Chinese Journal of Catalysis and is made available with permission of Dalian Institute of Chemical Physics, Chinese Academy of Sciences. application/pdf application/pdf |
| spellingShingle | Engineering::Chemical engineering CO₂ Splitting Iron‐Nickel Alloy Hu, Yue Wu, Jian Han, Yujia Xu, Weibin Zhang, Li Xia, Xue Huang, Chuande Zhu, Yanyan Tian, Ming Su, Yang Li, Lin Hou, Baolin Lin, Jian Liu, Wen Wang, Xiaodong Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title | Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title_full | Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title_fullStr | Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title_full_unstemmed | Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title_short | Intensified solar thermochemical CO₂ splitting over iron-based redox materials via perovskite-mediated dealloying-exsolution cycles |
| title_sort | intensified solar thermochemical co₂ splitting over iron based redox materials via perovskite mediated dealloying exsolution cycles |
| topic | Engineering::Chemical engineering CO₂ Splitting Iron‐Nickel Alloy |
| url | https://hdl.handle.net/10356/155655 |
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