In this work, second-generation Car–Parrinello-based mixed quantum-classical mechanics molecular dynamics simulations of small nanoparticles of NbP, NbAs, TaAs, and 1T-TaS₂ 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 explaining 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-TaS₂, 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 the proton reduction catalyst. Unexpectedly, the charge of the photosensitizer plays a decisive role for the photocatalytic performance.

中文翻译：

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Weyl半金属表面附近的水结构作为光催化质子还原的催化剂

在这项工作中，提出了第二代基于Car-Parrinello的混合量子古典力学的水中NbP，NbAs，TaAs和1T-TaS ₂纳米粒子的分子动力学模拟。前三种材料是拓扑Weyl半金属，最近发现它们是光催化水分解中的活性催化剂。这项研究的目的是将纳米粒子表面附近水结构中的电势差与这些材料在光诱导的质子还原中的光催化活性相关联。本文提供的结果可以解释这些Weyl半金属的催化活性：最具活性的材料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，以NbP为质子还原催化剂，对几种有机和金属有机光敏剂在氢气释放反应中的光催化活性进行了实验研究。出乎意料的是，光敏剂的电荷对光催化性能起决定性作用。