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Issue 20, 2019
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Origin of the overall water splitting activity of Ta3N5 revealed by ultrafast transient absorption spectroscopy

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Abstract

Tantalum nitride (Ta3N5) is one of the few visible light absorbing photocatalysts capable of overall water splitting (OWS), by which the evolution of both H2 and O2 is possible. Despite favourable energetics, realizing the OWS or efficient H2 evolution in Ta3N5 prepared by the nitridation of tantalum oxide (Ta2O5) or Ta foil remains a challenge even after 15 years of intensive research. Recently our group demonstrated OWS in Ta3N5 when prepared by the short time nitridation of potassium tantalate (KTaO3). To obtain a mechanistic insight on the role of Ta precursor and nitridation time in realizing OWS, ultrafast dynamics of electrons (3435 nm probe) and holes (545 nm probe) is investigated using transient absorption spectroscopy. Electrons decay majorly by trapping in Ta3N5 prepared by the nitridation of Ta2O5, which do not show OWS. However, OWS activity in Ta3N5 prepared by 0.25 hour nitridation of KTaO3 is particularly favoured by the virtually absent electron and hole trapping. On further increasing the nitridation time of KTaO3 from 0.25 to 10 hour, trapping of both electron and hole is enhanced which concurrently results in a reduction of the OWS activity. Insights from correlating the synthesis conditions—structural defects—carrier dynamics—photocatalytic activity is of importance in designing novel photocatalysts to enhance solar fuel production.

Graphical abstract: Origin of the overall water splitting activity of Ta3N5 revealed by ultrafast transient absorption spectroscopy

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Supplementary files

Article information


Submitted
15 Jan 2019
Accepted
25 Apr 2019
First published
25 Apr 2019

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2019,10, 5353-5362
Article type
Edge Article

Origin of the overall water splitting activity of Ta3N5 revealed by ultrafast transient absorption spectroscopy

D. H. K. Murthy, H. Matsuzaki, Z. Wang, Y. Suzuki, T. Hisatomi, K. Seki, Y. Inoue, K. Domen and A. Furube, Chem. Sci., 2019, 10, 5353
DOI: 10.1039/C9SC00217K

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