Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride.
JACS Au
; 4(5): 2019-2028, 2024 May 27.
Article
en En
| MEDLINE
| ID: mdl-38818073
ABSTRACT
Poly(triazine imide)·Li+Cl- (PTI/Li+Cl-) as one of the most reported crystalline carbon nitrides has shown exciting potential for photocatalysis. However, understanding the role of Li+/Cl- in the photoexcited charge transfer in the time and space of PTI is a challenging problem. Here, we have investigated the nonradiative charge recombination of series ion intercalated PTI systems (PTI/Li+X-, where X = F, Cl, Br, and I) by performing the ab initio nonadiabatic molecular dynamics simulations. The results indicate that the intercalated anions in PTI/Li+Cl- and PTI/Li+Br- have the potential to trap holes, separate the electrons and holes, and prolong the nonradiative electron-hole recombination. In particular, â¼70% of holes in PTI/Li+Cl- can transport among interlayers toward the {0001} planes, while most of the electrons are transferred to the {101Ì
0} planes, exhibiting different transport pathways and directions. Furthermore, PTI/Li+Cl- has an electron-hole recombination time as long as 136 ns, which explains its excellent optoelectronic properties. This work provides a theoretical baseline for the reported facet engineering improvement of crystalline carbon nitride for overall water splitting.
Texto completo:
1
Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
JACS Au
Año:
2024
Tipo del documento:
Article
Pais de publicación:
Estados Unidos