Exploring the Origins of Improved Photocurrent by Acidic Treatment for Quaternary Tantalum-Based Oxynitride Photoanodes on the Example of CaTaO2N

Quaternary tantalum-based oxynitrides ATa(O,N)(3),with electronic band gaps between 1.8 and 2.4 eV, are promising materials for photochemical water-splitting. The tailoring of their surface properties is a critical aspect to obtain efficient hole extraction. We report on the origin of improved photoelectrochemical (PEC) water oxidation by means of acidic treatment for this class of compounds on the example of cubic CaTaO2N particles. We address the effect of acidic treatment by using complementary physical characterization techniques, such as X-ray photoelectron spectroscopy, electrochemical impedance spectroscopy, H-1 and N-1 solid-state nuclear magnetic resonance (NMR) spectroscopy, electron microscopy, and electronic band structure calculations at the density functional theory level. In combination with PEC measurements, solid-state NMR indicates that the restructured surface displays a meaningfully higher concentration of terminating OH groups. Subsequent deposition of a nickel borate (NiBi;) catalyst on the acid-treated surface yields a higher percentual upsurge of photocurrent in comparison to pristine CaTaO2N. Our results highlight the application of solid-state NMR spectroscopy for understanding the semiconductor-catalyst interface in photochemical devices.

Jaworski, AleksanderStockholms universitet,Institutionen för material- och miljökemi (MMK)(Swepub:su)ajawo (author)
George, Janine (author)
Rokicinska, Anna (author)
Thersleff, ThomasStockholms universitet,Institutionen för material- och miljökemi (MMK)(Swepub:su)tther (author)
Budnyak, Tetyana M.Stockholms universitet,Institutionen för material- och miljökemi (MMK)(Swepub:su)tebu2966 (author)
Hautier, Geoffroy (author)
Pell, Andrew J.Stockholms universitet,Institutionen för material- och miljökemi (MMK)(Swepub:su)apell (author)
Dronskowski, Richard (author)
Kuśtrowski, Piotr (author)
Slabon, AdamStockholms universitet,Institutionen för material- och miljökemi (MMK)(Swepub:su)adsl1265 (author)
Stockholms universitetInstitutionen för material- och miljökemi (MMK) (creator_code:org_t)

In:The Journal of Physical Chemistry C: American Chemical Society (ACS)124:1, s. 152-1601932-74471932-7455

By the author/editor: Ma, Zili; Jaworski, Aleksa ...; George, Janine; Rokicinska, Anna; Thersleff, Thoma ...; Budnyak, Tetyana ...; show more...; Hautier, Geoffro ...; Pell, Andrew J.; Dronskowski, Ric ...; Kuśtrowski, Piot ...; Slabon, Adam; show less...

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