Engineered disorder in CO2 photocatalysis
Abstract Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sod...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2022-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-022-34798-1 |
| _version_ | 1797778872189583360 |
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| author | Zhao Li Chengliang Mao Qijun Pei Paul N. Duchesne Teng He Meikun Xia Jintao Wang Lu Wang Rui Song Feysal M. Ali Débora Motta Meira Qingjie Ge Kulbir Kaur Ghuman Le He Xiaohong Zhang Geoffrey A. Ozin |
| author_facet | Zhao Li Chengliang Mao Qijun Pei Paul N. Duchesne Teng He Meikun Xia Jintao Wang Lu Wang Rui Song Feysal M. Ali Débora Motta Meira Qingjie Ge Kulbir Kaur Ghuman Le He Xiaohong Zhang Geoffrey A. Ozin |
| author_sort | Zhao Li |
| collection | DOAJ |
| description | Abstract Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sodium and TiO2 forms a core-shell c-TiO2@a-TiO2-x(OH)y heterostructure, comprised of HO-Ti-[O]-Ti surface frustrated Lewis pairs (SFLPs) embedded in an amorphous shell surrounding a crystalline core, which enables a new genre of chemical reactivity. Specifically, these SFLPs heterolytically dissociate dihydrogen at room temperature to form charge-balancing protonated hydroxyl groups and hydrides at unsaturated titanium surface sites, which display high reactivity towards CO2 reduction. This crystalline-amorphous heterostructure also boosts light absorption, charge carrier separation and transfer to SFLPs, while prolonged carrier lifetimes and photothermal heat generation further enhance reactivity. The collective results of this study motivate a general approach for catalytically generating sustainable chemicals and fuels through engineered disorder in heterogeneous CO2 photocatalysts. |
| first_indexed | 2024-03-12T23:22:46Z |
| format | Article |
| id | doaj.art-e6b9fb098ee74692b3845e52e6974dac |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-12T23:22:46Z |
| publishDate | 2022-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-e6b9fb098ee74692b3845e52e6974dac2023-07-16T11:20:27ZengNature PortfolioNature Communications2041-17232022-11-0113111110.1038/s41467-022-34798-1Engineered disorder in CO2 photocatalysisZhao Li0Chengliang Mao1Qijun Pei2Paul N. Duchesne3Teng He4Meikun Xia5Jintao Wang6Lu Wang7Rui Song8Feysal M. Ali9Débora Motta Meira10Qingjie Ge11Kulbir Kaur Ghuman12Le He13Xiaohong Zhang14Geoffrey A. Ozin15Institute of Functional Nano & Soft Materials (FUNSOM), Soochow UniversitySolar Fuels Group, Department of Chemistry, University of TorontoDalian Institute of Chemical Physics, Chinese Academy of SciencesDepartment of Chemistry, Queen’s UniversityDalian Institute of Chemical Physics, Chinese Academy of SciencesSolar Fuels Group, Department of Chemistry, University of TorontoDalian Institute of Chemical Physics, Chinese Academy of SciencesThe Chinese University of Hong Kong, ShenzhenInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow UniversitySolar Fuels Group, Department of Chemistry, University of TorontoCLS@APS, Advanced Photon Source, Argonne National LaboratoryDalian Institute of Chemical Physics, Chinese Academy of SciencesInstitut National de la Recherche Scientifique, Centre Énergie, Matériaux et TélécommunicationsInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow UniversityInstitute of Functional Nano & Soft Materials (FUNSOM), Soochow UniversitySolar Fuels Group, Department of Chemistry, University of TorontoAbstract Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sodium and TiO2 forms a core-shell c-TiO2@a-TiO2-x(OH)y heterostructure, comprised of HO-Ti-[O]-Ti surface frustrated Lewis pairs (SFLPs) embedded in an amorphous shell surrounding a crystalline core, which enables a new genre of chemical reactivity. Specifically, these SFLPs heterolytically dissociate dihydrogen at room temperature to form charge-balancing protonated hydroxyl groups and hydrides at unsaturated titanium surface sites, which display high reactivity towards CO2 reduction. This crystalline-amorphous heterostructure also boosts light absorption, charge carrier separation and transfer to SFLPs, while prolonged carrier lifetimes and photothermal heat generation further enhance reactivity. The collective results of this study motivate a general approach for catalytically generating sustainable chemicals and fuels through engineered disorder in heterogeneous CO2 photocatalysts.https://doi.org/10.1038/s41467-022-34798-1 |
| spellingShingle | Zhao Li Chengliang Mao Qijun Pei Paul N. Duchesne Teng He Meikun Xia Jintao Wang Lu Wang Rui Song Feysal M. Ali Débora Motta Meira Qingjie Ge Kulbir Kaur Ghuman Le He Xiaohong Zhang Geoffrey A. Ozin Engineered disorder in CO2 photocatalysis Nature Communications |
| title | Engineered disorder in CO2 photocatalysis |
| title_full | Engineered disorder in CO2 photocatalysis |
| title_fullStr | Engineered disorder in CO2 photocatalysis |
| title_full_unstemmed | Engineered disorder in CO2 photocatalysis |
| title_short | Engineered disorder in CO2 photocatalysis |
| title_sort | engineered disorder in co2 photocatalysis |
| url | https://doi.org/10.1038/s41467-022-34798-1 |
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