Department of Chemistry, University of Crete, Heraklion 71003, Greece.
Department of Chemistry, University of South Florida, Tampa, Florida 33620, United States.
Inorg Chem. 2023 Apr 10;62(14):5496-5504. doi: 10.1021/acs.inorgchem.2c04483. Epub 2023 Mar 28.
We utilized the platform of MOFs for the synthesis of two new water-stable compounds based on amide functionalized trigonal tritopic organic linkers HBTBTB (L1), HBTCTB (L2) and Al metal ions, namely, and . The mesoporous material exhibits an impressive methane (CH) uptake at high pressures and ambient temperature. The corresponding values of 192 cm (STP) cm, 0.254 g g at 100 bar, and 298 K are among the highest reported for mesoporous MOFs, while the gravimetric and volumetric working capacities (between 80 bar and 5 bar) can be well compared to the best MOFs for CH storage. Furthermore, at 298 K and 50 bar, adsorbs 50 wt % (304 cm (STP) cm) CO, values among the best recorded for CO storage using porous materials. To gain insight into the mechanism accounting for the resultant enhanced CH storage capacity, theoretical calculations were performed, revealing the presence of strong CH adsorption sites near the amide groups. Our work demonstrates that amide functionalized mesoporous -MOFs can be valuable for the design of versatile coordination compounds with CH and CO storage capacities comparable to ultra-high surface area microporous MOFs.
我们利用 MOFs 平台，基于酰胺官能化三角三聚体有机连接体 HBTBTB（L1）、HBTCTB（L2）和 Al 金属离子，合成了两种新的水稳定化合物，即 和 。介孔材料在高压和环境温度下表现出令人印象深刻的甲烷（CH）吸收。在 100 巴和 298 K 下，相应的 192 cm（STP）cm、0.254 g g 值是介孔 MOFs 中报道的最高值之一，而重量和体积工作容量（在 80 巴到 5 巴之间）可以与 CH 储存的最佳 MOFs 相媲美。此外，在 298 K 和 50 巴下， 吸附 50 wt%（304 cm（STP）cm）CO，这是使用多孔材料储存 CO 时记录的最佳值之一。为了深入了解导致 CH 储存容量增强的机制，进行了理论计算，结果表明酰胺基团附近存在强 CH 吸附位。我们的工作表明，酰胺官能化介孔 -MOFs 可用于设计具有 CH 和 CO 储存能力的多功能配合物，其能力可与超高表面积微孔 MOFs 相媲美。
