Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes
Summary: Singlet oxygen (1O2) shows great potential for selective degradation of dyes in environmental remediation of wastewater. In this study, we showcased that 1O2 can be effectively generated from an anion complex composed of deprotonated hexafluoroisopropanol anion ([HFIP-H]‒) with hydroperoxyl...
| Main Authors: | , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2023-08-01
|
| Series: | iScience |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2589004223013834 |
| _version_ | 1827894557336928256 |
|---|---|
| author | Jia Han Lei Wang Wenjin Cao Qinqin Yuan Xiaoguo Zhou Shilin Liu Xue-Bin Wang |
| author_facet | Jia Han Lei Wang Wenjin Cao Qinqin Yuan Xiaoguo Zhou Shilin Liu Xue-Bin Wang |
| author_sort | Jia Han |
| collection | DOAJ |
| description | Summary: Singlet oxygen (1O2) shows great potential for selective degradation of dyes in environmental remediation of wastewater. In this study, we showcased that 1O2 can be effectively generated from an anion complex composed of deprotonated hexafluoroisopropanol anion ([HFIP-H]‒) with hydroperoxyl radical (⋅HO2) via ultraviolet (UV) photodetachment. Electronic structure calculations and cryogenic negative ion photoelectron spectroscopy unveil critical proton transfer upon complex formation and electron ejection, effectively photoconverting prevalent triplet ground state 3O2 to long-lived excited 1O2, stabilized by nearby HFIP. Inspired by this spectroscopic study, a novel “photogeneration” strategy is proposed to produce 1O2 with the incorporation of atmospheric O2 and HFIP, acting as a catalyst. Conceptually, the designed catalytic cycle upon UV irradiation and electron injection is able to achieve different degradations of dye molecules in a controllable fashion from decolorization to complete mineralization, shedding new light on potential water purification. |
| first_indexed | 2024-03-12T22:09:03Z |
| format | Article |
| id | doaj.art-6aab7f25db7447c5859e4dc0d363ff7a |
| institution | Directory Open Access Journal |
| issn | 2589-0042 |
| language | English |
| last_indexed | 2024-03-12T22:09:03Z |
| publishDate | 2023-08-01 |
| publisher | Elsevier |
| record_format | Article |
| series | iScience |
| spelling | doaj.art-6aab7f25db7447c5859e4dc0d363ff7a2023-07-24T04:10:48ZengElsevieriScience2589-00422023-08-01268107306Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyesJia Han0Lei Wang1Wenjin Cao2Qinqin Yuan3Xiaoguo Zhou4Shilin Liu5Xue-Bin Wang6Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. ChinaHefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. ChinaPhysical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USADepartment of Chemistry, Anhui University, Hefei, Anhui 230601, P.R. ChinaHefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China; Corresponding authorHefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. ChinaPhysical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA; Corresponding authorSummary: Singlet oxygen (1O2) shows great potential for selective degradation of dyes in environmental remediation of wastewater. In this study, we showcased that 1O2 can be effectively generated from an anion complex composed of deprotonated hexafluoroisopropanol anion ([HFIP-H]‒) with hydroperoxyl radical (⋅HO2) via ultraviolet (UV) photodetachment. Electronic structure calculations and cryogenic negative ion photoelectron spectroscopy unveil critical proton transfer upon complex formation and electron ejection, effectively photoconverting prevalent triplet ground state 3O2 to long-lived excited 1O2, stabilized by nearby HFIP. Inspired by this spectroscopic study, a novel “photogeneration” strategy is proposed to produce 1O2 with the incorporation of atmospheric O2 and HFIP, acting as a catalyst. Conceptually, the designed catalytic cycle upon UV irradiation and electron injection is able to achieve different degradations of dye molecules in a controllable fashion from decolorization to complete mineralization, shedding new light on potential water purification.http://www.sciencedirect.com/science/article/pii/S2589004223013834Density functional theoryModeling chemical reactivity |
| spellingShingle | Jia Han Lei Wang Wenjin Cao Qinqin Yuan Xiaoguo Zhou Shilin Liu Xue-Bin Wang Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes iScience Density functional theory Modeling chemical reactivity |
| title | Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| title_full | Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| title_fullStr | Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| title_full_unstemmed | Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| title_short | Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| title_sort | photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes |
| topic | Density functional theory Modeling chemical reactivity |
| url | http://www.sciencedirect.com/science/article/pii/S2589004223013834 |
| work_keys_str_mv | AT jiahan photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT leiwang photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT wenjincao photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT qinqinyuan photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT xiaoguozhou photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT shilinliu photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes AT xuebinwang photogenerationofsingletoxygencatalyzedbyhexafluoroisopropanolforselectivedegradationofdyes |