Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning
Photocatalytic conversion of carbon dioxide (CO2) into value-added fuels is a vastly promising anthropogenic chemical carbon cycle to combat the greenhouse effect while meeting the ever-increasing energy demand. Recently, lead-based halide perovskites have demonstrated great potential in various app...
| Main Authors: | , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Online Access: | https://hdl.handle.net/10356/170640 |
| _version_ | 1811684454179012608 |
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| author | Lee, Jiale Chong, Wei-Kean Kok, Steven Hao Wan Ng, Boon-Junn Kong, Xin Ying Chai, Siang-Piao Tan, Lling-Lling |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Lee, Jiale Chong, Wei-Kean Kok, Steven Hao Wan Ng, Boon-Junn Kong, Xin Ying Chai, Siang-Piao Tan, Lling-Lling |
| author_sort | Lee, Jiale |
| collection | NTU |
| description | Photocatalytic conversion of carbon dioxide (CO2) into value-added fuels is a vastly promising anthropogenic chemical carbon cycle to combat the greenhouse effect while meeting the ever-increasing energy demand. Recently, lead-based halide perovskites have demonstrated great potential in various applications including photochemical reduction of CO2. However, in view of lead toxicity, the exploration of a lead-free alternative is crucial for long term application. Herein, a series of lead-free mixed halide perovskites Cs3Sb2ClxBr9−x (0 ≤ x ≤ 9) is prepared via a facile antisolvent recrystallization technique, where the incorporation of a secondary halide enhances the charge transfer and separation while allowing precise tuning of bandgap between 2.59 and 2.90 eV. Theoretical calculations further reveal that the formation of mixed Cl/Br halides engenders favorable charge redistribution due to lower octahedral distortion, which in turn strengthens CO2 adsorption and activation. Under visible light illumination, the optimal dual halide perovskite, Cs3Sb2Cl4Br5 manifests substantial twofold and fourfold enhancements of CH4 yield over the single halide perovskite, Cs3Sb2Br9 and Cs3Sb2Cl9, respectively. In brief, this study provides a compelling demonstration of lead-free mixed halide perovskites for photocatalytic CO2 reduction, and it is anticipated to drive further application of perovskite-based photocatalysts toward a diverse range of artificial photoredox reactions. |
| first_indexed | 2024-10-01T04:28:53Z |
| format | Journal Article |
| id | ntu-10356/170640 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:28:53Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1706402023-09-29T15:31:46Z Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning Lee, Jiale Chong, Wei-Kean Kok, Steven Hao Wan Ng, Boon-Junn Kong, Xin Ying Chai, Siang-Piao Tan, Lling-Lling School of Chemistry, Chemical Engineering and Biotechnology Engineering::Chemical engineering CO2 Reduction Halide Tuning Photocatalytic conversion of carbon dioxide (CO2) into value-added fuels is a vastly promising anthropogenic chemical carbon cycle to combat the greenhouse effect while meeting the ever-increasing energy demand. Recently, lead-based halide perovskites have demonstrated great potential in various applications including photochemical reduction of CO2. However, in view of lead toxicity, the exploration of a lead-free alternative is crucial for long term application. Herein, a series of lead-free mixed halide perovskites Cs3Sb2ClxBr9−x (0 ≤ x ≤ 9) is prepared via a facile antisolvent recrystallization technique, where the incorporation of a secondary halide enhances the charge transfer and separation while allowing precise tuning of bandgap between 2.59 and 2.90 eV. Theoretical calculations further reveal that the formation of mixed Cl/Br halides engenders favorable charge redistribution due to lower octahedral distortion, which in turn strengthens CO2 adsorption and activation. Under visible light illumination, the optimal dual halide perovskite, Cs3Sb2Cl4Br5 manifests substantial twofold and fourfold enhancements of CH4 yield over the single halide perovskite, Cs3Sb2Br9 and Cs3Sb2Cl9, respectively. In brief, this study provides a compelling demonstration of lead-free mixed halide perovskites for photocatalytic CO2 reduction, and it is anticipated to drive further application of perovskite-based photocatalysts toward a diverse range of artificial photoredox reactions. Published version This research project was funded by the Ministry of Higher Education (MOHE) Malaysia under the Fundamental Research Grant Scheme (FRGS) - (Ref No.: FRGS/1/2020/TK0/MUSM/02/1). This work was also supported by High-Performance Computer (HPC) Platform from Monash University Malaysia. 2023-09-25T02:41:47Z 2023-09-25T02:41:47Z 2023 Journal Article Lee, J., Chong, W., Kok, S. H. W., Ng, B., Kong, X. Y., Chai, S. & Tan, L. (2023). Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning. Advanced Functional Materials. https://dx.doi.org/10.1002/adfm.202303430 1616-301X https://hdl.handle.net/10356/170640 10.1002/adfm.202303430 2-s2.0-85162011465 en Advanced Functional Materials © 2023 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. application/pdf |
| spellingShingle | Engineering::Chemical engineering CO2 Reduction Halide Tuning Lee, Jiale Chong, Wei-Kean Kok, Steven Hao Wan Ng, Boon-Junn Kong, Xin Ying Chai, Siang-Piao Tan, Lling-Lling Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title | Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title_full | Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title_fullStr | Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title_full_unstemmed | Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title_short | Mixed halide formation in lead-free antimony-based halide perovskite for boosted CO₂ photoreduction: beyond band gap tuning |
| title_sort | mixed halide formation in lead free antimony based halide perovskite for boosted co₂ photoreduction beyond band gap tuning |
| topic | Engineering::Chemical engineering CO2 Reduction Halide Tuning |
| url | https://hdl.handle.net/10356/170640 |
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