摘要
The design and construction of chemical or physical adsorbents for clean energy storage(such as hydrogen) and carbon dioxide capture is vital to addressing the persisting challenges in global energy issues and environmental sustainability. Various porous materials have been developed over the past decades. Among them, metal–organic frameworks(MOFs), an emerging unique class of crystalline solid-state materials, show great promise owing to their adjustable chemical functionality, structural diversity, and ease of functionalization via pre-and/or post-synthesis. Typically, MOFs are built by the self-assembly of metal ions or clusters and polytopic bridging ligands under solvothermal conditions. The incorporation of accessible nitrogen-donor groups, such as pyridine, imidazole, and tetrazole, into the pore walls of porous materials can dramatically affect the gas uptake capacity and selectivity of the materials, especially for CO_2 capture on account of the dipole-quadrupole interactions between the polarizable CO_2 molecule and the accessible nitrogen site. Such approach is strategically important for developing a low-carbon future by increasing the capacity of selective CO_2 capture and by enhancing the storage capacity of clean energy source, such as H_2. However, competitive coordination of these Lewis basic nitrogen sites with metal ions or clusters is a great challenge in direct synthesis of MOFs. Herein, we have utilized click reaction to design and synthesize a series of carboxylates ligands possessing nitrogen-rich triaolze groups(Scheme 1). Furthermore, MOFs are constructed by these ligands.
The design and construction of chemical or physical adsorbents for clean energy storage(such as hydrogen) and carbon dioxide capture is vital to addressing the persisting challenges in global energy issues and environmental sustainability. Various porous materials have been developed over the past decades. Among them, metal–organic frameworks(MOFs), an emerging unique class of crystalline solid-state materials, show great promise owing to their adjustable chemical functionality, structural diversity, and ease of functionalization via pre-and/or post-synthesis. Typically, MOFs are built by the self-assembly of metal ions or clusters and polytopic bridging ligands under solvothermal conditions. The incorporation of accessible nitrogen-donor groups, such as pyridine, imidazole, and tetrazole, into the pore walls of porous materials can dramatically affect the gas uptake capacity and selectivity of the materials, especially for CO_2 capture on account of the dipole-quadrupole interactions between the polarizable CO_2 molecule and the accessible nitrogen site. Such approach is strategically important for developing a low-carbon future by increasing the capacity of selective CO_2 capture and by enhancing the storage capacity of clean energy source, such as H_2. However, competitive coordination of these Lewis basic nitrogen sites with metal ions or clusters is a great challenge in direct synthesis of MOFs. Herein, we have utilized click reaction to design and synthesize a series of carboxylates ligands possessing nitrogen-rich triaolze groups(Scheme 1). Furthermore, MOFs are constructed by these ligands.
引文
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