It is an emerging trend to develop synthetic ammonia via nitrogen reduction reaction(NRR) by using simple, economical and efficient catalysts under mild conditions. Due to the intrinsic rich-functional groups of the surface, its versatile tailorability and the true stability among all the two-dimensional materials, reduced graphene oxide (rGO) is drawing a rising attention of researchers to the NRR application. However, due to the hydrophobicity of C and hydrophilicity of oxygen-containing groups of rGO, the interface dynamics between rGO surface and N₂ and H₂O molecules, which are two basic precursors for catalytic NRR are still unclear up to date. Herein, we propose to explore this problem by constructing a hierarchical model for rGO-N₂/H₂O interface interaction and conducting molecular dynamics (MD) simulation at ambient conditions. We find a way to tune the function groups to maximize the adsorption of N₂ and H₂O molecules at the same time. H₂O molecules are more likely to form hydrogen bonds with oxygen-containing groups of rGO in the near range. While in the remote region, N₂ molecules tend to form non-bonding interactions with pure C atoms without oxygen-containing groups of rGO. These results will provide theoretical guidance for NRR based on rGO and rGO based materials.

通过在温和条件下使用简单，经济和高效的催化剂，通过氮还原反应（NRR）来开发合成氨是一种新兴趋势。由于表面固有的丰富官能团，其通用的可定制性以及所有二维材料之间的真正稳定性，还原氧化石墨烯（rGO）引起了研究人员对NRR应用的关注。然而，由于rGO的C的疏水性和含氧基团的亲水性，至今仍不清楚rGO表面与作为催化NRR的两个基本前体的N ₂和H ₂ O分子之间的界面动力学。本文中，我们建议通过构建rGO-N ₂ / H ₂的层次模型来探索此问题。在环境条件下进行O界面相互作用并进行分子动力学（MD）模拟。我们找到了一种调节功能基团以同时最大化N ₂和H ₂ O分子吸附的方法。H ₂ O分子更可能与rGO的含氧基团在近距离形成氢键。在偏远地区，N ₂分子倾向于与没有rGO含氧基团的纯C原子形成非键相互作用。这些结果将为基于rGO和基于rGO的材料的NRR提供理论指导。