发表机构
Sardar Vallabhbhai National Institute of Technology（萨达尔·瓦拉巴伊·帕特尔国家理工学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
该研究通过第一性原理计算发现h-Be3N2单层是带隙1.74 eV的直接带隙半导体，具有合适带边位置，可在中性和碱性环境实现光催化分解水，在酸性或中性条件下需外加电位，是潜在的光催化制氢材料。
AI 中文摘要
在本工作中，我们利用基于第一性原理的密度泛函理论，系统研究了二维h-Be3N2单层在分解水应用中的结构稳定性、电子性质和光催化性能。基于PBE泛函的电子结构计算表明，h-Be3N2是一种直接带隙半导体，带隙值为1.74 eV，非常适合可见光驱动的光催化。此外，带边排列显示h-Be3N2具有合适的氧化还原电位，有利于在中性和碱性环境中实现整体光催化分解水。相反，在酸性条件下，价带位置足以支持析氧反应（OER），从而导致光阴极行为。在中性pH下，施加0.77 V的外加电位仍可实现析氢反应（HER）过程。对于析氧反应，仅在强碱性条件下热力学上有利，而在中性pH下需要0.43 V的外加电位来促进反应。这些结果清楚地强调了溶液pH和光生载流子对h-Be3N2单层光催化效率的显著影响。此外，对H覆盖度的研究表明，附着在表面的H数量对h-Be3N2中析氢反应的效率有相当大的影响。h-Be3N2单层有利的光催化能力表明，它可能是未来太阳能驱动绿色制氢的可行选择，并可能通过促进有效和可持续的氢气生产，帮助实现国家绿色氢能使命的目标。
英文摘要
In this work, we have systematically investigated the structural stability, electronic properties, and photocatalytic performance of the 2D h-Be3N2 monolayer for water splitting application, utilizing a first-principles density functional theory. Electronic structure calculations based on the PBE functional reveal that h-Be3N2 is a direct band-gap semiconductor with a band gap value of 1.74 eV, making it well suited for visible-light-driven photocatalysis. Furthermore, the alignment of band-edges illustrates that h-Be3N2 has suitable redox potential that facilitate overall photocatalytic water splitting in neutral and alkaline environment. Conversely, in acidic condition, the position of valence band is an adequate to enable the OER, thereby leading to photocathodic behavior. At neutral pH, the HER process is still possible with the application of an external potential of 0.77 V. For the OER process, it is thermodynamically favourable only under strongly alkaline conditions, while an external potential of 0.43 V is needed to promote the reaction at neutral pH. These results clearly underscore the significant impact of solution pH and photogenerated charge carriers on the photocatalytic effectiveness of the h-Be3N2 monolayer. Furthermore, the study of H coverage indicates that the amount of H that adheres to the surface has a considerable impact on the efficiency of the HER in h-Be3N2. The favourable photocatalytic capabilities of the h-Be3N2 monolayer imply that it might be a viable option for upcoming solar-powered green hydrogen generation and may assist in realizing the goals of the National Green Hydrogen Mission by facilitating effective and sustainable hydrogen production.
Comments32 pages, 10 figures
