Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 29, Issue 11, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201808389
Keywords
defect chemistry; defect engineering; material defect; nonstoichiometric defect; solar energy conversion
Categories
Funding
- National Key Research and Development Program of China [2018YFA0209303]
- National Natural Science Foundation of China [U1663228, 21473090]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
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Nonstoichiometric defects, as manifested by slight deviation of elemental compositions from chemical formulas, are common yet highly important in solid materials. Oxynitrides with a relatively large O/N ratio variation are theoretically predicted to change their electronic structures and charge transport behaviors with these nonstoichiometric defects. However, little experimental effort is devoted to understanding the impact of such nonstoichiometric defects regarding varied O/N ratios in oxynitrides for solar water splitting. The main reason is the lack of suitable oxynitride research models for aforementioned nonstoichiometric defect study without interference from other factors. Using TaON as a prototypical material, finely tuned O/N ratios can dramatically influence its photoresponse. In-depth analysis further reveals a significant impact of nonstoichiometric defects (O/N ratios) on TaON's charge carrier densities, charge separation, and transport. Finally, manipulating nonstoichiometric defects of O/N ratios demonstrates its ability to control the space charge layer width and film conductivity of TaON photoanodes for high efficiency water splitting. Therefore, a fine understanding and control of nonstoichiometric defects would be highly important for future development of high efficiency oxynitrides for water splitting.
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