We introduce the first mechanochemical cyclotrimerization of nitriles, a facile strategy for synthesizing triazine‐containing molecules and materials, overcoming challenges related to carbonization and solubility. Conducting this solid‐state approach in a mixer ball mill with 4‐Methylbenzonitrile, we synthesize Tris(4‐methylphenyl)‐1,3,5‐triazine quantitatively in as little as 90 minutes. Just as fast, this mechanochemical method facilitates the synthesis of the covalent triazine framework CTF‐1 using 1,4 Dicyanobenzene. Material characterization confirms its porous (650m²g‐1) and crystalline nature. Adjusting the induced mechanical energy allows control over the obtained stacking conformation of the resulting CTFs ‐ from a staggered AB arrangement to an eclipsed AA stacking conformation. Finally, a substrate scope demonstrates the versatility of this approach, successfully yielding various CTFs.

中文翻译：

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机械化学环三聚：具有可调堆叠模式的共价有机框架的多功能工具

我们引入了第一个腈的机械化学环三聚，这是一种合成含三嗪分子和材料的简便策略，克服了与碳化和溶解度相关的挑战。通过在混合球磨机中使用 4-甲基苯甲腈进行这种固态方法，我们在短短 90 分钟内定量合成了三(4-甲基苯基)-1,3,5-三嗪。同样快，这种机械化学方法有利于使用 1,4 二氰基苯合成共价三嗪骨架 CTF-1。材料特性证实了其多孔（650m²g-1）和结晶性质。调整感应机械能可以控制所得 CTF 的堆叠构象——从交错的 AB 排列到重叠的 AA 堆叠构象。最后，底物示波器展示了这种方法的多功能性，成功产生了各种 CTF。