A Porous Crystalline Nitrone‐Linked Covalent Organic Framework**
A Porous Crystalline Nitrone‐Linked Covalent Organic Framework**
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多孔结晶硝酮 - 连接共价有机框架**
DOI：
10.1002/anie.202307674
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Yaghi, Omar M.
中科院分区：
文献类型：
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作者：
Kurandina, Daria;Huang, Banruo;Xu, Wentao;Hanikel, Nikita;Darù, Andrea;Stroscio, Gautam D.;Wang, Kaiyu;Gagliardi, Laura;Toste, F. Dean;Yaghi, Omar M.
在此，我们报道了通过将N,N',N',N'''-(乙烯-1,1,2,2-四基四(苯-4,1-二基))四(羟胺)和对苯二甲醛结合，合成了硝酮连接的共价有机框架COF-115。 缩聚反应。硝酮官能团的形成通过 13C 同位素标记的 COF-115 的固态 13C 多交叉偏振魔角旋转 NMR 光谱和傅里叶变换红外光谱证实。通过低压 N2、CO2 和 H2 吸附实验评估 COF-115 的永久孔隙率。 COF-115和等网状亚胺连接的COF的水蒸气和二氧化碳吸附分析表明N-氧化物基多孔材料在大气水收集和二氧化碳捕获应用中具有优越的潜力。密度泛函理论计算为了解这些 COF 的吸附特性之间的差异提供了有价值的见解。最后，成功证明了 COF-115 与相关酰胺连接材料的光诱导重排。
Herein, we report the synthesis of a nitrone‐linked covalent organic framework, COF‐115, by combiningN,N′,N′,N′′′‐(ethene‐1, 1, 2, 2‐tetrayltetrakis(benzene‐4, 1‐diyl))tetrakis(hydroxylamine) and terephthaladehyde via a polycondensation reaction. The formation of the nitrone functionality was confirmed by solid‐state13C multi cross‐polarization magic angle spinning NMR spectroscopy of the13C‐isotope‐labeled COF‐115 and Fourier‐transform infrared spectroscopy. The permanent porosity of COF‐115 was evaluated through low‐pressure N2, CO2, and H2sorption experiments. Water vapor and carbon dioxide sorption analysis of COF‐115 and the isoreticular imine‐linked COF indicated a superior potential ofN‐oxide‐based porous materials for atmospheric water harvesting and CO2capture applications. Density functional theory calculations provided valuable insights into the difference between the adsorption properties of these COFs. Lastly, photoinduced rearrangement of COF‐115 to the associated amide‐linked material was successfully demonstrated.