Suppression of charge carrier recombination in a Ta3N5 photoanode via defect regulation: a theoretical investigation

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F24%3A10489917" target="_blank" >RIV/00216208:11310/24:10489917 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=x4uTDoHenu" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=x4uTDoHenu</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/d4ta01693a" target="_blank" >10.1039/d4ta01693a</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Suppression of charge carrier recombination in a Ta3N5 photoanode via defect regulation: a theoretical investigation

Popis výsledku v původním jazyce

Defect-induced charge carrier recombination in a photoanode significantly restricts the efficiency of solar-driven water splitting. By systematically investigating the photoexcited charge carrier recombination dynamics of Ta3N5 with intrinsic defects, charge states, oxygen (O) impurities, and metal doping based on density functional theory (DFT) calculations and nonadiabatic molecular dynamics (NAMD) simulations, we propose two strategies to mitigate defect-induced charge carrier recombination: ionizing nitrogen (N) vacancies and magnesium (Mg) doping. Our results show that tantalum (Ta) reduction induced by N vacancies is the primary factor in reducing the carrier lifetime of the Ta3N5 photoanode. Ionizing N vacancies and Mg doping can tune the charges of reduced Ta species near the N vacancies, thus extending the recombination lifetime. By contrast, charge-balanced metal and O impurities co-doping in Ta3N5 photoanodes cannot significantly increase the lifetime. Our investigation sheds new light on understanding the charge carrier recombination mechanism and provides dependable strategies to improve the water-splitting performance of the Ta3N5 photoanode.

Název v anglickém jazyce

Suppression of charge carrier recombination in a Ta3N5 photoanode via defect regulation: a theoretical investigation

Popis výsledku anglicky

Defect-induced charge carrier recombination in a photoanode significantly restricts the efficiency of solar-driven water splitting. By systematically investigating the photoexcited charge carrier recombination dynamics of Ta3N5 with intrinsic defects, charge states, oxygen (O) impurities, and metal doping based on density functional theory (DFT) calculations and nonadiabatic molecular dynamics (NAMD) simulations, we propose two strategies to mitigate defect-induced charge carrier recombination: ionizing nitrogen (N) vacancies and magnesium (Mg) doping. Our results show that tantalum (Ta) reduction induced by N vacancies is the primary factor in reducing the carrier lifetime of the Ta3N5 photoanode. Ionizing N vacancies and Mg doping can tune the charges of reduced Ta species near the N vacancies, thus extending the recombination lifetime. By contrast, charge-balanced metal and O impurities co-doping in Ta3N5 photoanodes cannot significantly increase the lifetime. Our investigation sheds new light on understanding the charge carrier recombination mechanism and provides dependable strategies to improve the water-splitting performance of the Ta3N5 photoanode.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2024

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Materials Chemistry A

ISSN

2050-7488

e-ISSN

2050-7496

Svazek periodika

12

Číslo periodika v rámci svazku

26

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

8

Strana od-do

15922-15929

Kód UT WoS článku

001234661700001

EID výsledku v databázi Scopus

2-s2.0-85194969996