Two‐dimensional covalent organic frameworks (2D‐COFs) have recently emerged as fascinating scaffolds for solar‐to‐chemical energy conversion because of their customizable structures and functionalities. Herein, two tris(triazolo)triazine‐based COF materials (namely COF‐JLU51 and COF‐JLU52) featuring large surface area, high crystallinity, excellent stability and photoelectric properties were designed and constructed for the first time. Remarkably, COF‐JLU51 gave an outstanding H2O2 production rate of over 4200 µmol g−1 h−1 with excellent reusability in pure water and O2 under one standard sun light, that higher than its isomorphic COF‐JLU52 and most of the reported metal‐free materials, owing to its superior generation, separation and transport of photogenerated carriers. Experimental and theoretical researches prove that the photocatalytic process undergoes a combination of indirect 2e− O2 reduction reaction (ORR) and 4e− H2O oxidation reaction (WOR). Specifically, an ultrahigh yield of 7624.7 µmol g−1 h−1 with apparent quantum yield of 18.2% for COF‐JLU52 was achieved in a 1:1 ratio of benzyl alcohol and water system. This finding contributes novel, nitrogen‐rich and high‐quality tris(triazolo)triazine‐based COF materials, and also designate their bright future in photocatalytic solar transformations.

中文翻译：

---

基于三（三唑）三嗪的共价有机框架用于高效光催化生产过氧化氢


二维共价有机框架（2D-COF）最近因其可定制的结构和功能而成为太阳能到化学能转换的令人着迷的支架。在此，首次设计并构建了两种三（三唑）三嗪基COF材料（即COF-JLU51和COF-JLU52），它们具有大表面积、高结晶度、优异的稳定性和光电性能。值得注意的是，COF-JLU51 在一个标准太阳光下的纯水和 O2 中具有超过 4200 µmol g−1 h−1 的出色的 H2O2 产率，并且具有出色的可重复使用性，高于其同构 COF-JLU52 和大多数报道的金属 -自由材料，由于其卓越的光生载流子生成、分离和传输能力。实验和理论研究证明，光催化过程经历了间接2e−O2还原反应（ORR）和4e−H2O氧化反应（WOR）的组合。具体而言，COF-JLU52在苯甲醇和水比例为1:1的体系中实现了7624.7 µmol g−1 h−1的超高产率，表观量子产率为18.2%。这一发现提供了新型、富氮、高质量的三（三唑）三嗪基COF材料，也预示着它们在光催化太阳能转化方面的光明前景。