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We have developed a new penternary wurtzitic nitride system Li1-xZnxGe2-xGaxN3 (0 < x < 1) by hybridizing LiGe2N3 and ZnGeGaN3. Fairly stoichiometric fine powder samples were synthesized by the reduction-nitridation process at 900 degree C. While the end member LiGe2N3 possessed a relatively large band gap of 4.16 eV, the band gap of the developed penternary system varied in a broad range of 3.81-3.10 eV, showing promising responsivity to the solar spectrum. The crystal structure of LiGe2N3 was precisely determined by time-of-flight neutron powder diffraction for the first time, revealing the complete ordering of Li and Ge in the Cmc21 structure. The structural evolution from the completely ordered LiGe2N3 to the fully disordered ZnGeGaN3 was quantitatively analyzed by Rietveld refinement based on a partially disordered Cmc21 model, and the obtained results were also supported by 71Ga solid-state NMR spectroscopy.
The synthesized Li1-xZnxGe2-xGaxN3 powder samples exhibited photocatalytic activities for the water reduction and oxidation reactions under solar-light irradiation, with the H2 evolution rate of 0.3-59.0 micro mol/h and the O2 evolution rate of 3.1-296.2 micro mol/h, depending on the composition. Stable solar hydrogen generation of up to 48 h was demonstrated by the x = 0.80 sample, with the total amount of H2 evolved over 1.6 mmol and the external quantum efficiency of 2.1%.

権利情報:

• In Copyright
  This document is the Accepted Manuscript version of a Published Work that appeared in final form in Inorganic Chemistry, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.inorgchem.4c01294

キーワード: Nitride, Photocatalyst, Photocatalysis, Hydrogen, Wurtzite

刊行年月日: 2024-07-01

出版者: American Chemical Society (ACS)

掲載誌:

• Inorganic Chemistry (ISSN: 00201669) vol. 63 issue. 26

研究助成金:

• Japan Society for the Promotion of Science 21K04913

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4566

公開URL: https://doi.org/10.1021/acs.inorgchem.4c01294

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更新時刻: 2025-06-14 08:30:31 +0900

MDRでの公開時刻: 2025-06-14 08:22:20 +0900