Surface Hydrogen Bond-Induced Oxygen Vacancies of TiO2 for Two-Electron Molecular Oxygen Activation and Efficient NO Oxidation
Defect engineering can provide a feasible approach to achieving ambient molecular oxygen activation. However, conventional surface defects (e.g., oxygen vacancies, OVs), featured with the coordinatively unsaturated metal sites, often favor the reduction of O2 to •O2- rather than O22- via two-electron transfer, hindering the efficient pollutant removal with high electron utilization. Herein, we demonstrate that this bottleneck can be well discharged by modulating the electronic structure of OVs via phosphorization. As a proof of concept, TiO2 nanoparticles are adopted as a model material for NaH2PO2 (HP) modification, in which HP induces the formation of OVs via weakening the Ti-O bonds through the hydrogen bond interactions. Additionally, the formed Ti-O-P covalent bond refines the electronic structure of OVs, which enables rapid electron transfer for two-electron molecular oxygen activation. As exemplified by NO oxidation, HP-modified TiO2 with abundant OVs achieved complete NO removal with high selectivity for benign nitrate, superior to that of pristine TiO2. This study highlights a promising approach to regulate the O2 activation via an electronic structure modulation and provides fresh insights into the rational design of a photocatalyst for environmental remediation.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:57 |
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| Enthalten in: |
Environmental science & technology - 57(2023), 48 vom: 05. Dez., Seite 20400-20409 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Shang, Huan [VerfasserIn] |
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| Links: |
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| Themen: |
15FIX9V2JP |
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| Anmerkungen: |
Date Completed 07.12.2023 Date Revised 07.12.2023 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/acs.est.3c06593 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM364791373 |
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| 520 | |a Defect engineering can provide a feasible approach to achieving ambient molecular oxygen activation. However, conventional surface defects (e.g., oxygen vacancies, OVs), featured with the coordinatively unsaturated metal sites, often favor the reduction of O2 to •O2- rather than O22- via two-electron transfer, hindering the efficient pollutant removal with high electron utilization. Herein, we demonstrate that this bottleneck can be well discharged by modulating the electronic structure of OVs via phosphorization. As a proof of concept, TiO2 nanoparticles are adopted as a model material for NaH2PO2 (HP) modification, in which HP induces the formation of OVs via weakening the Ti-O bonds through the hydrogen bond interactions. Additionally, the formed Ti-O-P covalent bond refines the electronic structure of OVs, which enables rapid electron transfer for two-electron molecular oxygen activation. As exemplified by NO oxidation, HP-modified TiO2 with abundant OVs achieved complete NO removal with high selectivity for benign nitrate, superior to that of pristine TiO2. This study highlights a promising approach to regulate the O2 activation via an electronic structure modulation and provides fresh insights into the rational design of a photocatalyst for environmental remediation | ||
| 650 | 4 | |a Journal Article | |
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| 650 | 4 | |a O2 activation | |
| 650 | 4 | |a defect engineering | |
| 650 | 4 | |a electronic structure modulation | |
| 650 | 4 | |a hydrogen bond | |
| 650 | 4 | |a photocatalysis | |
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| 700 | 1 | |a Jia, Hongbao |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Wenbin |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Shuangjun |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Qing |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Qingyu |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Chi |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Yuxin |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Yongjie |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Pengpeng |e verfasserin |4 aut | |
| 700 | 1 | |a He, Yucheng |e verfasserin |4 aut | |
| 700 | 1 | |a Xiao, Shuning |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Ding |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Dieqing |e verfasserin |4 aut | |
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