First-Principles DFT Insights into the Stabilization of Zinc Diphosphide (ZnP 2 ) Nanocrystals via Surface Functionalization by 4-Aminothiophenol for Photovoltaic Applications
First-Principles DFT Insights into the Stabilization of Zinc Diphosphide (ZnP 2 ) Nanocrystals via Surface Functionalization by 4-Aminothiophenol for Photovoltaic Applications
复制标题
第一原理 DFT 洞察通过 4-氨基苯硫酚表面功能化稳定二磷化锌 (ZnP 2 ) 纳米晶体的光伏应用
DOI：
10.1021/acsaem.1c03804
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发表时间：
2022
影响因子：
6.4
通讯作者：
Farkaš B
中科院分区：
文献类型：
--
作者：
Farkaš B
人们对磷化锌化合物作为高效太阳能吸收剂的兴趣重新兴起，引发了人们越来越多的努力来提高其在潮湿和富氧条件下的稳定性。尽管有机功能化被认为是钝化磷化锌纳米粒子的一种有前途的策略，但仍然缺乏对二磷化锌 (ZnP2) 表面吸附过程和结构的基本原子水平见解。本研究通过密度泛函理论计算研究了4-氨基苯硫酚与单斜ZnP2低米勒指数表面之间的相互作用。双齿吸附模式，其中 4-氨基苯硫酚通过 Zn-N 和 Zn-S 键通过其两个官能团结合，预计是最强的相互作用形式，并且发现单层功能化 ZnP2 表面在富含吸附物的条件下高度稳定。还讨论了功能化过程中 ZnP2 纳米晶平衡形态的变化以及湿度的影响。研究结果预计将有助于光伏（PV）器件中ZnP2基材料的合理设计。
The resurgence of interest in zinc phosphide compounds as efficient solar absorbers has initiated increasing efforts to improve their stability under humid and oxygen-rich conditions. Although organic functionalization has been suggested as a promising strategy to passivate zinc phosphide nanoparticles, fundamental atomic-level insights into the adsorption processes and structures at zinc diphosphide (ZnP2) surfaces are still lacking. In this study, the interactions between 4-aminothiophenol and the low-Miller index surfaces of monoclinic ZnP2have been investigated by means of density functional theory calculations. A bidentate adsorption mode, in which 4-aminothiophenol binds through both its functional groups via Zn–N and Zn–S bonds, was predicted to be the strongest form of interaction, and monolayer-functionalized ZnP2surfaces were found to be highly stable under adsorbate-rich conditions. Changes in the equilibrium morphology of ZnP2nanocrystallites upon functionalization and effects of humidity are also discussed. The results are expected to contribute toward the rational design of ZnP2-based materials for photovoltaic (PV) devices.