The efficiency of photocatalytic nitrogen reduction reactions (NRRs) faces significant challenges due to the need for effective activation of the NN bond and efficient multi-electron/proton transfer. A novel Gd-doped and Mo₁₅S₁₉-loaded g-C₃N₄ nanorod (GdC₃N₄/Mo₁₅S₁₉) is promoted in this work. The experimental results show that the GdC₃N₄/Mo₁₅S₁₉ composite exhibits remarkable visible-light-driven photocatalytic ammonia production (407.51 μmol g⁻¹ h⁻¹, 33 times that of g-C₃N₄), which is attributed to the promoted multiple electron transfer by in-built Gd³⁺ redox centers and increased Mo active sites by loading of Mo₁₅S₁₉. Calculations using Density Functional Theory (DFT) show that Mo₁₅S₁₉ loading also helps to effectively activate the NN bond, which accelerates the NRR's start. The synergistic effect of Gd doping and Mo₁₅S₁₉ loading lowers the Gibbs free energy of intermediates, enhancing the overall photocatalytic efficiency. This work provides a viable approach to the construction of multistage structures in the photocatalytic NRR that incorporates multiple electron transfer and N₂ activation effects.

中文翻译：

---

Gd 掺杂 g-C3N4/Mo15S19 复合材料的多级构建实现了 N2 活化和多电子转移，从而增强了光催化氮还原反应


由于需要有效激活 N N 键和高效的多电子/质子转移，光催化氮还原反应 （NRR） 的效率面临重大挑战。这项工作推广了一种新型的 Gd 掺杂和 Mo₁₅S₁₉ 负载的 g-C₃N₄ 纳米棒 （GdC₃N₄/Mo₁₅S₁₉）。实验结果表明，GdC₃N₄/Mo₁₅S₁₉ 复合材料表现出显著的可见光驱动光催化氨产生 （407.51 μmol ^{g-1 h-1}，是 g-C₃N₄ 的 33 倍），这归因于内置 Gd ^{促进了多电子转移通过}加载 Mo₁₅S₁₉ 获得 3+ 氧化还原中心和增加的 Mo 活性位点。使用密度泛函理论 （DFT） 的计算表明，Mo₁₅S₁₉ 负载也有助于有效激活 N N 键，从而加速 NRR 的启动。Gd 掺杂和 Mo₁₅S₁₉ 负载的协同作用降低了中间体的吉布斯自由能，提高了整体光催化效率。这项工作为在光催化 NRR 中构建多级结构提供了一种可行的方法，该方法结合了多电子转移和 N₂ 活化效应。