Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride,JACS Au

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Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride
JACS Au ( IF 8.5 ) Pub Date : 2024-05-13 , DOI: 10.1021/jacsau.4c00216
Xu Cai ₁ , Wei Lin _{1,

2}

Affiliation

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, ∼70% of holes in PTI/Li⁺Cl^– can transport among interlayers toward the {0001} planes, while most of the electrons are transferred to the {101̅0} 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.

中文翻译：

氯离子诱导晶体氮化碳中光生电子和空穴的空间分离和长复合时间

聚（三嗪酰亚胺）·Li ⁺ Cl ^– (PTI/Li ⁺ Cl ^– ) 作为报道最多的晶体氮化碳之一，显示出令人兴奋的光催化潜力。然而，理解Li ⁺ / ^Cl-在PTI时空光生电荷转移中的作用是一个具有挑战性的问题。在这里，我们通过从头算非绝热分子动力学模拟研究了串联离子插层 PTI 系统（PTI/Li ⁺ X ^– ，其中 X = F、Cl、Br 和 I）的非辐射电荷重组。结果表明，PTI/Li ⁺ Cl ^-和 PTI/Li ⁺ Br ^-中的插层阴离子具有捕获空穴、分离电子和空穴并延长非辐射电子-空穴复合的潜力。特别是，PTI/Li ⁺ Cl ^–中~70%的空穴可以在层间向{0001}面传输，而大部分电子则转移到{101̅0}面，表现出不同的传输路径和方向。此外，PTI/Li ⁺ Cl ^–的电子-空穴复合时间长达136 ns，这解释了其优异的光电性能。这项工作为所报道的用于整体水分解的结晶氮化碳的面工程改进提供了理论基线。

更新日期：2024-05-13

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