论文标题
韦基半含量的水结构作为光催化质子还原的催化剂
Water structure near the surface of Weyl semimetals as catalysts in photocatalytic proton reduction
论文作者
论文摘要
在这项工作中，提出了基于第二代CAR-PARRINELLO的QM/mm分子动力学模拟NBP，NBA，TAA和1T-TAS $ _2 $的水的小纳米颗粒。前三种材料是拓扑Weyl半含量，最近发现它们是光催化水分裂中的活性催化剂。这项研究的目的是将纳米颗粒表面附近水结构的潜在差异与这些材料在光诱导的质子还原中的光催化活性相关联。本文介绍的结果允许解释这些Weyl半含量的催化活性：最活跃的材料NBP在纳米颗粒表面附近表现出特别低的水配位，而对于1T-TAS $ _2 $，具有最低的催化活性，表面的水结构最有序。另外，用NBP作为质子还原催化剂研究了氢进化反应中几种有机和金属光敏剂的光催化活性。出乎意料的是，光敏剂的电荷对于光催化性能起决定性作用。
In this work, second-generation Car-Parrinello-based QM/MM molecular dynamics simulations of small nanoparticles of NbP, NbAs, TaAs and 1T-TaS$_2$ in water are presented. The first three materials are topological Weyl semimetals, which were recently discovered to be active catalysts in photocatalytic water splitting. The aim of this research was to correlate potential differences in the water structure in the vicinity of the nanoparticle surface with the photocatalytic activity of these materials in light induced proton reduction. The results presented herein allow to explain the catalytic activity of these Weyl semimetals: the most active material, NbP, exhibits a particularly low water coordination near the surface of the nanoparticle, whereas for 1T-TaS$_2$, with the lowest catalytic activity, the water structure at the surface is most ordered. In addition, the photocatalytic activity of several organic and metalorganic photosensitizers in the hydrogen evolution reaction was experimentally investigated with NbP as proton reduction catalyst. Unexpectedly, the charge of the photosensitizer plays a decisive role for the photocatalytic performance.
