In Situ Modulation of A-Site Vacancies in LaMnO3.15 Perovskite for Surface Lattice Oxygen Activation and Boosted Redox Reactions
© 2021 Wiley-VCH GmbH..
Modulation of A-site defects is crucial to the redox reactions on ABO3 perovskites for both clean air application and electrochemical energy storage. Herein we report a scalable one-pot strategy for in situ regulation of La vacancies (VLa ) in LaMnO3.15 by simply introducing urea in the traditional citrate process, and further reveal the fundamental relationship between VLa creation and surface lattice oxygen (Olatt ) activation. The underlying mechanism is shortened Mn-O bonds, decreased orbital ordering, promoted MnO6 bending vibration and weakened Jahn-Teller distortion, ultimately realizing enhanced Mn-3d and O-2p orbital hybridization. The LaMnO3.15 with optimized VLa exhibits order of magnitude increase in toluene oxidation and ca. 0.05 V versus RHE (reversible hydrogen electrode) increase of half-wave potential in oxygen reduction reaction (ORR). The reported strategy can benefit the development of novel defect-meditated perovskites in both heterocatalysis and electrocatalysis.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2021 |
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| Erschienen: |
2021 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:60 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - 60(2021), 51 vom: 13. Dez., Seite 26747-26754 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Liu, Xiaoqing [VerfasserIn] |
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| Links: |
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| Themen: |
A-site defects |
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| Anmerkungen: |
Date Revised 07.12.2021 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/anie.202111610 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM332057615 |
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| 100 | 1 | |a Liu, Xiaoqing |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a In Situ Modulation of A-Site Vacancies in LaMnO3.15 Perovskite for Surface Lattice Oxygen Activation and Boosted Redox Reactions |
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| 500 | |a Date Revised 07.12.2021 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2021 Wiley-VCH GmbH. | ||
| 520 | |a Modulation of A-site defects is crucial to the redox reactions on ABO3 perovskites for both clean air application and electrochemical energy storage. Herein we report a scalable one-pot strategy for in situ regulation of La vacancies (VLa ) in LaMnO3.15 by simply introducing urea in the traditional citrate process, and further reveal the fundamental relationship between VLa creation and surface lattice oxygen (Olatt ) activation. The underlying mechanism is shortened Mn-O bonds, decreased orbital ordering, promoted MnO6 bending vibration and weakened Jahn-Teller distortion, ultimately realizing enhanced Mn-3d and O-2p orbital hybridization. The LaMnO3.15 with optimized VLa exhibits order of magnitude increase in toluene oxidation and ca. 0.05 V versus RHE (reversible hydrogen electrode) increase of half-wave potential in oxygen reduction reaction (ORR). The reported strategy can benefit the development of novel defect-meditated perovskites in both heterocatalysis and electrocatalysis | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a A-site defects | |
| 650 | 4 | |a ABO3 | |
| 650 | 4 | |a catalytic oxidation | |
| 650 | 4 | |a oxygen reduction reaction | |
| 650 | 4 | |a surface lattice oxygen | |
| 700 | 1 | |a Mi, Jinxing |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Lin |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Haiyan |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Jun |e verfasserin |4 aut | |
| 700 | 1 | |a Ding, Yun |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Jianqiang |e verfasserin |4 aut | |
| 700 | 1 | |a He, Minghua |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Zisha |e verfasserin |4 aut | |
| 700 | 1 | |a Xiong, Shangchao |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Qinfang |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Yuefeng |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Zhong-Shuai |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Jianjun |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Junhua |e verfasserin |4 aut | |
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