Undoped Layered Perovskite Oxynitride Li2LaTa2O6N for Photocatalytic CO2 Reduction with Visible Light

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Abstract
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 500 nm. As opposed to well‐known 3D oxynitride perovskites, Li2LaTa2O6N supported by a binuclear RuII complex was capable of stably and selectively converting CO2 into formate under visible light (λ>400 nm). 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.
Funding Information
  • Japan Society for the Promotion of Science (JP16H06438, JP16H06439, JP16H06440, JP16H06441, JP16K21724, JP17H05491, JP17H05478, JP16H06130, JP17K17762, JP16KK0097, JP16J10084, JP17J06914, JP17J03705)
  • Japan Science and Technology Corporation (JPMJPR16NA, JPMJCR13L1, Support Program for Starting Up Innovation Hub MI2I)
  • Ministry of Education, Culture, Sports, Science and Technology (hp170269, hp180175)
  • Toyota Motor Corporation
  • Air Force Office of Scientific Research (AFOSR-AOARD/FA2386-17-1-4049)

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