Photocatalytic nitrogen (N2) fixation is a promising strategy for green ammonia (NH3) synthesis. However, the design of catalysts possessing high nitrogen adsorption capacity and efficient N2 dissociation remains a significant challenge, owing to the poor solubility of N2 in aqueous solutions coupled with its high chemical stability. Herein, we prepared Ru-TiO2 with metal lattice strain and applied it to a gas–solid two-phase system (G-S). Compared to the conventional gas–liquid-solid three-phase system (G-L-S), the G-S system can effectively enhance N2 adsorption and shorten the diffusive mass transfer path. Additionally, Ru-TiO2 demonstrates improved N2 adsorption capacity and activation efficiency, giving the maximum NH3 production rate of 38.7 μmol g−1 h−1, which is about four times higher than that in the G-L-S system. Density functional theory results demonstrate that N2 adsorption and activation are optimized over the lattice-strained Ru surface. This work provides an innovative approach to developing advanced photocatalysts and NRR systems.

中文翻译：

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制备 Ru 诱导晶格应变 TiO2 增强气固反应体系中光催化固氮作用


光催化氮 （N₂） 固定是绿氨 （NH₃） 合成的一种很有前途的策略。然而，由于 N₂ 在水溶液中的溶解度差，加上其化学稳定性高，因此设计具有高氮吸附能力和高效 N₂ 解离的催化剂仍然是一个重大挑战。在此，我们制备了具有金属晶格应变的 Ru-TiO₂ 并将其应用于气固两相系统 （G-S）。与传统的气-液-固三相体系 （G-L-S） 相比，G-S 体系可以有效增强 N₂ 吸附并缩短扩散传质路径。此外，Ru-TiO₂ 表现出更高的 N₂ 吸附能力和活化效率，NH₃ 的最大产生速率为 38.7 μmol ^{g-1 h-1}，大约是 G-L-S 系统的四倍。密度泛函理论结果表明，N₂ 吸附和活化在晶格应变 Ru 表面上得到优化。这项工作为开发先进的光催化剂和 NRR 系统提供了一种创新方法。