Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 27, Pages 8154-8158Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201803931
Keywords
CO2 reduction; oxynitride; perovskites; photocatalysis; visible light
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Funding
- JSPS [JP16H06438, JP16H06439, JP16H06440, JP16H06441, JP17H05491, JP16K21724, JP17H05478]
- JST [JP16H06130, JP17K17762, JP16KK0097, JPMJPR16NA, JPMJCR13L1]
- Noguchi Institute
- Murata Research Foundation
- JSPS Fellowship for Young Scientists [JP16J10084, JP17J06914, JP17J03705]
- FLAGSHIP2020 (MEXT) [hp170269, hp180175]
- Toyota Motor Corporation
- I-O DATA Foundation
- Air Force Office of Scientific Research [AFOSR-AOARD/FA2386-17-1-4049]
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Oxynitrides are promising visible-light-responsive photocatalysts, but their structures are almost confined with three-dimensional (3D) structures such as perovskites. A phase-pure Li2LaTa2O6N with a layered perovskite structure was successfully prepared by thermal ammonolysis of a lithium-rich oxide precursor. Li2LaTa2O6N exhibited high crystallinity and visible-light absorption up to 500nm. As opposed to well-known 3D oxynitride perovskites, Li2LaTa2O6N supported by a binuclear Ru-II complex was capable of stably and selectively converting CO2 into formate under visible light (>400nm). Transient absorption spectroscopy indicated that, as compared to 3D oxynitrides, Li2LaTa2O6N possesses a lower density of mid-gap states that work as recombination centers of photogenerated electron/hole pairs, but a higher density of reactive electrons, which is responsible for the higher photocatalytic performance of this layered oxynitride.
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