论文标题
无定形固体的精确电子结构：揭开颜色起源和黑色钛的光催化
Precise electronic structures of amorphous solids: unraveling the color origin and photocatalysis of black titania
论文作者
论文摘要
通过有效的催化剂分裂的水代表了40年内碳中立性的最终解决方案。为了实现这一目标，无定形的光催化剂因其有前途的表现而闻名。其中，最著名的是黑色二氧化钛（无定形tiox，x <2）。然而，尽管对黑二钛进行了大量研究，但其颜色起源，结构 - 特性关系和光催化机制仍然是热门辩论的话题，这主要是由于难以计算其精确的电子结构。在这里，使用摘要分子动力学模拟，我们报告了黑钛的精确电子结构，并进一步揭示了在非晶化和还原后共价化合物的电子结构的通用进化模式。此外，首次模拟了共催化剂原子（例如PT）对无定形物质的表面吸附：无序的表面可以轻松适应共催化剂原子，而扩展的电子状态则有助于将光诱导的电子和孔分离出来，对氢的分离，对氢的进化有益。这项研究阐明了无定形催化剂的起作用，并提供了增强其性能的实用指导。
Water splitting through efficient catalysts represents an ultimate solution for carbon neutrality within 40 years. To achieve this goal, amorphous photocatalysts are noted for their promising performances. Among them, the best known is black titania (amorphous TiOx, x < 2). However, despite the large number of studies on black titania, its color origin, structure-property relationship, and photocatalytic mechanism remain a topic of hot debate, largely due to the difficulty to calculate its precise electronic structure. Here, using ab initio molecular dynamics simulations, we report the precise electronic structures of black titania and further reveal the generic evolution pattern of the electronic structures of covalent compounds upon amorphization and reduction. Moreover, surface adsorption of the co-catalyst atoms (e.g., Pt) on amorphous substances is simulated for the first time: the disordered surface enables easy accommodation of the co-catalyst atoms, while the extended electronic states facilitate the separation of photo-induced electrons and holes, beneficial for hydrogen evolution. This study elucidates the workings of amorphous catalysts and offers practical guidance for enhancing their performances.
