Band Gap Adjustment in Perovskite-type Eu 1-x Ca x TiO 3 via Ammonolysis

Widenmeyer, Marc; Kohler, Tobias; Samolis, Margarita; Denko, Alexandra T.  De; Xiao, Xingxing; Xie, Wenjie; Osterloh, Frank E.; Weidenkaff, Anke

doi:10.1515/zpch-2019-1429

Title: Band Gap Adjustment in Perovskite-type Eu _1-x Ca _x TiO ₃ via Ammonolysis

Journal Article · Tue Dec 10 00:00:00 EST 2019 · Zeitschrift fuer Physikalische Chemie

DOI:https://doi.org/10.1515/zpch-2019-1429· OSTI ID:1802732

Widenmeyer, Marc ^[1]; Kohler, Tobias ^[2]; Samolis, Margarita ^[2]; Denko, Alexandra T. De ^[3]; Xiao, Xingxing ^[1]; Xie, Wenjie ^[1]; Osterloh, Frank E. ^[3]; Weidenkaff, Anke ^[4]

Univ. of Stuttgart (Germany). Inst. for Materials Science; Technische Univ. Darmstadt (Germany). Inst. of Materials Science
Univ. of Stuttgart (Germany). Inst. for Materials Science
Univ. of California, Davis, CA (United States). Dept. of Chemistry
Univ. of Stuttgart (Germany). Inst. for Materials Science; Technische Univ. Darmstadt (Germany). Inst. of Materials Science; Fraunhofer Institute Materials Recycling and Resource Strategies IWKS, Hanau, (Germany)

Perovskite-type oxynitridesAB(O,N)₃are potential candidates for photoelectrode materials in solar water splitting. A drawback of these materials is their low sintering tendency resulting in low electrical conductivities. Typically, they are prepared by ammonia treatment of insulating, wide band gap oxides. In this study, we propose an approach starting from small band gap oxides Eu_1-xCa_xTiO_3-_δand then widen the band gaps in a controlled way by ammonolysis and partial Ca²⁺substitution. Both together induced a distortion of the octahedral network and dilution of the Eu4fand N2plevels in the valence band. The effect is the stronger the more Ca²⁺is present. Within the series of samples, Eu_0.4Ca_0.6Ti(O,N)₃had the most suitable optical band gap (E_G≈ 2.2 eV) for water oxidation. However, its higher Eu content compared to Eu_0.1Ca_0.9Ti(O,N)₃slowed down the charge carrier dynamics due to enhanced trapping and recombination as expressed by large accumulation (τ_on) and decay (τ_off) times of the photovoltage of up to 109 s and 486 s, respectively. In contrast, the highly Ca²⁺-substituted samples (x≥ 0.7) were more prone to formation of TiN and oxygen vacancies also leading to Ti³⁺donor levels below the conduction band. Therefore, a precise control of the ammonolysis temperature is essential, since even small amounts of TiN can suppress the photovoltage generation by fast recombination processes. Water oxidation tests on Eu_0.4Ca_0.6Ti(O,N)₃revealed a formation of 7.5 μmol O₂from 50 mg powder together with significant photocorrosion of the bare material. Combining crystal structure, chemical composition, and optical and electronical band gap data, a first simplified model of the electronical band structure of Eu_1-xCa_xTi(O,N)₃could be proposed.

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Research Organization:: Univ. of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0015329

OSTI ID:: 1802732

Journal Information:: Zeitschrift fuer Physikalische Chemie, Vol. 234, Issue 5; ISSN 0942-9352

Publisher:: de GruyterCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Band Gap Adjustment in Perovskite-type Eu 1-x Ca x TiO 3 via Ammonolysis

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Title: Band Gap Adjustment in Perovskite-type Eu _1-x Ca _x TiO ₃ via Ammonolysis