Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism
Deciphering the metal-support interaction-oriented catalysis on millimeter-scaled catalysts is highly desirable yet remains scarce in Fenton-like catalysis. Herein, we fine-tune the support-surface reconstruction of Co2AlO4 on γ-Al2O3 millispheres and reveal the origins of its activity in peroxymono...
| Main Authors: | , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/172878 |
| _version_ | 1826110992841441280 |
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| author | Zhu, Min-Ping Yang, Jia-Cheng E. Guan, Daqin Yuan, Baoling Duan, Xiaoguang Sun, Darren Delai Sun, Chenghua Wang, Shaobin Fu, Ming-Lai |
| author2 | School of Civil and Environmental Engineering |
| author_facet | School of Civil and Environmental Engineering Zhu, Min-Ping Yang, Jia-Cheng E. Guan, Daqin Yuan, Baoling Duan, Xiaoguang Sun, Darren Delai Sun, Chenghua Wang, Shaobin Fu, Ming-Lai |
| author_sort | Zhu, Min-Ping |
| collection | NTU |
| description | Deciphering the metal-support interaction-oriented catalysis on millimeter-scaled catalysts is highly desirable yet remains scarce in Fenton-like catalysis. Herein, we fine-tune the support-surface reconstruction of Co2AlO4 on γ-Al2O3 millispheres and reveal the origins of its activity in peroxymonosulfate activation by nuclear magnetic resonance and X-ray photoelectron/adsorption spectroscopy. Calcination of γ-Al2O3 supports rearranged their surface octahedral, tetrahedral and pentacoordinate Al3+. The reconstructed tetrahedral and pentacoordinate Al3+ as binding sites regulated the formation of Co2AlO4 with coordinated Co3+/Co2+ redox centers via strong metal-support interactions. The activities of tailored Co2AlO4 @Al2O3 millispheres in activating peroxymonosulfate follow different binomial models, highly relying on their Co3+/Co2+ ratio, contents of lattice O and pentacoordinate Al3+. The Co-O-Al bonds endow the millimeter-scaled Co2AlO4 @Al2O3 with robust catalytic activity, stability and reusability. The exposed Co2AlO4 (200) surface is responsible for the decomposition of PMS into produce SO4•[sbnd] and 1O2 as the dominant oxidants for water detoxification. |
| first_indexed | 2024-10-01T02:43:19Z |
| format | Journal Article |
| id | ntu-10356/172878 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T02:43:19Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1728782023-12-27T06:47:24Z Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism Zhu, Min-Ping Yang, Jia-Cheng E. Guan, Daqin Yuan, Baoling Duan, Xiaoguang Sun, Darren Delai Sun, Chenghua Wang, Shaobin Fu, Ming-Lai School of Civil and Environmental Engineering Engineering::Environmental engineering Metal-Support Interaction Support-Surface Reconstruction Deciphering the metal-support interaction-oriented catalysis on millimeter-scaled catalysts is highly desirable yet remains scarce in Fenton-like catalysis. Herein, we fine-tune the support-surface reconstruction of Co2AlO4 on γ-Al2O3 millispheres and reveal the origins of its activity in peroxymonosulfate activation by nuclear magnetic resonance and X-ray photoelectron/adsorption spectroscopy. Calcination of γ-Al2O3 supports rearranged their surface octahedral, tetrahedral and pentacoordinate Al3+. The reconstructed tetrahedral and pentacoordinate Al3+ as binding sites regulated the formation of Co2AlO4 with coordinated Co3+/Co2+ redox centers via strong metal-support interactions. The activities of tailored Co2AlO4 @Al2O3 millispheres in activating peroxymonosulfate follow different binomial models, highly relying on their Co3+/Co2+ ratio, contents of lattice O and pentacoordinate Al3+. The Co-O-Al bonds endow the millimeter-scaled Co2AlO4 @Al2O3 with robust catalytic activity, stability and reusability. The exposed Co2AlO4 (200) surface is responsible for the decomposition of PMS into produce SO4•[sbnd] and 1O2 as the dominant oxidants for water detoxification. The authors acknowledge the support from National Natural Science Foundation of China (Grant Nos. 51978638 and 51808524), National Science Foundation of Fujian Province (2020J01120), Youth Innovation Promotion Association of Chinese Academy of Sciences (2023320), Scientific Research Founds of Huaqiao University (20BS109) and China Scholarship Council (202004910092). 2023-12-27T06:47:23Z 2023-12-27T06:47:23Z 2023 Journal Article Zhu, M., Yang, J. E., Guan, D., Yuan, B., Duan, X., Sun, D. D., Sun, C., Wang, S. & Fu, M. (2023). Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism. Applied Catalysis B: Environmental, 329, 122570-. https://dx.doi.org/10.1016/j.apcatb.2023.122570 0926-3373 https://hdl.handle.net/10356/172878 10.1016/j.apcatb.2023.122570 2-s2.0-85150811350 329 122570 en Applied Catalysis B: Environmental © 2023 Elsevier B.V. All rights reserved. |
| spellingShingle | Engineering::Environmental engineering Metal-Support Interaction Support-Surface Reconstruction Zhu, Min-Ping Yang, Jia-Cheng E. Guan, Daqin Yuan, Baoling Duan, Xiaoguang Sun, Darren Delai Sun, Chenghua Wang, Shaobin Fu, Ming-Lai Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title | Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title_full | Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title_fullStr | Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title_full_unstemmed | Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title_short | Surface Al and Co coordination for peroxymonosulfate activation: identification and mechanism |
| title_sort | surface al and co coordination for peroxymonosulfate activation identification and mechanism |
| topic | Engineering::Environmental engineering Metal-Support Interaction Support-Surface Reconstruction |
| url | https://hdl.handle.net/10356/172878 |
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