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Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy

Tantalum nitride (Ta(3)N(5)) is one of the few visible light absorbing photocatalysts capable of overall water splitting (OWS), by which the evolution of both H(2) and O(2) is possible. Despite favourable energetics, realizing the OWS or efficient H(2) evolution in Ta(3)N(5) prepared by the nitridat...

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Autores principales: Murthy, Dharmapura H. K., Matsuzaki, Hiroyuki, Wang, Zheng, Suzuki, Yohichi, Hisatomi, Takashi, Seki, Kazuhiko, Inoue, Yasunobu, Domen, Kazunari, Furube, Akihiro
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6540954/
https://www.ncbi.nlm.nih.gov/pubmed/31191893
http://dx.doi.org/10.1039/c9sc00217k
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author Murthy, Dharmapura H. K.
Matsuzaki, Hiroyuki
Wang, Zheng
Suzuki, Yohichi
Hisatomi, Takashi
Seki, Kazuhiko
Inoue, Yasunobu
Domen, Kazunari
Furube, Akihiro
author_facet Murthy, Dharmapura H. K.
Matsuzaki, Hiroyuki
Wang, Zheng
Suzuki, Yohichi
Hisatomi, Takashi
Seki, Kazuhiko
Inoue, Yasunobu
Domen, Kazunari
Furube, Akihiro
author_sort Murthy, Dharmapura H. K.
collection PubMed
description Tantalum nitride (Ta(3)N(5)) is one of the few visible light absorbing photocatalysts capable of overall water splitting (OWS), by which the evolution of both H(2) and O(2) is possible. Despite favourable energetics, realizing the OWS or efficient H(2) evolution in Ta(3)N(5) prepared by the nitridation of tantalum oxide (Ta(2)O(5)) or Ta foil remains a challenge even after 15 years of intensive research. Recently our group demonstrated OWS in Ta(3)N(5) when prepared by the short time nitridation of potassium tantalate (KTaO(3)). 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 Ta(3)N(5) prepared by the nitridation of Ta(2)O(5), which do not show OWS. However, OWS activity in Ta(3)N(5) prepared by 0.25 hour nitridation of KTaO(3) is particularly favoured by the virtually absent electron and hole trapping. On further increasing the nitridation time of KTaO(3) 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.
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spelling pubmed-65409542019-06-12 Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy Murthy, Dharmapura H. K. Matsuzaki, Hiroyuki Wang, Zheng Suzuki, Yohichi Hisatomi, Takashi Seki, Kazuhiko Inoue, Yasunobu Domen, Kazunari Furube, Akihiro Chem Sci Chemistry Tantalum nitride (Ta(3)N(5)) is one of the few visible light absorbing photocatalysts capable of overall water splitting (OWS), by which the evolution of both H(2) and O(2) is possible. Despite favourable energetics, realizing the OWS or efficient H(2) evolution in Ta(3)N(5) prepared by the nitridation of tantalum oxide (Ta(2)O(5)) or Ta foil remains a challenge even after 15 years of intensive research. Recently our group demonstrated OWS in Ta(3)N(5) when prepared by the short time nitridation of potassium tantalate (KTaO(3)). 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 Ta(3)N(5) prepared by the nitridation of Ta(2)O(5), which do not show OWS. However, OWS activity in Ta(3)N(5) prepared by 0.25 hour nitridation of KTaO(3) is particularly favoured by the virtually absent electron and hole trapping. On further increasing the nitridation time of KTaO(3) 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. Royal Society of Chemistry 2019-04-25 /pmc/articles/PMC6540954/ /pubmed/31191893 http://dx.doi.org/10.1039/c9sc00217k Text en This journal is © The Royal Society of Chemistry 2019 http://creativecommons.org/licenses/by/3.0/ This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0)
spellingShingle Chemistry
Murthy, Dharmapura H. K.
Matsuzaki, Hiroyuki
Wang, Zheng
Suzuki, Yohichi
Hisatomi, Takashi
Seki, Kazuhiko
Inoue, Yasunobu
Domen, Kazunari
Furube, Akihiro
Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title_full Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title_fullStr Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title_full_unstemmed Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title_short Origin of the overall water splitting activity of Ta(3)N(5) revealed by ultrafast transient absorption spectroscopy
title_sort origin of the overall water splitting activity of ta(3)n(5) revealed by ultrafast transient absorption spectroscopy
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6540954/
https://www.ncbi.nlm.nih.gov/pubmed/31191893
http://dx.doi.org/10.1039/c9sc00217k
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