Department of Chemistry, University of Chicago , 929 East 57th Street, Chicago, Illinois 60637, United States.
J Am Chem Soc. 2014 Sep 24;136(38):13182-5. doi: 10.1021/ja507947d. Epub 2014 Sep 15.
A robust and porous Zr metal-organic framework, sal-MOF, of UiO topology was synthesized using a salicylaldimine (sal)-derived dicarboxylate bridging ligand. Postsynthetic metalation of sal-MOF with iron(II) or cobalt(II) chloride followed by treatment with NaBEt3H in THF resulted in Fe- and Co-functionalized MOFs (sal-M-MOF, M = Fe, Co) which are highly active solid catalysts for alkene hydrogenation. Impressively, sal-Fe-MOF displayed very high turnover numbers of up to 145000 and was recycled and reused more than 15 times. This work highlights the unique opportunity of developing MOF-based earth-abundant catalysts for sustainable chemical synthesis.
使用源自水杨醛亚胺(sal)的二羧酸桥联配体合成了具有 UiO 拓扑结构的坚固多孔 Zr 金属有机骨架 sal-MOF。通过后合成的金属化与氯化铁(II)或氯化钴(II)随后用 NaBEt3H 在 THF 中处理,得到了 Fe 和 Co 功能化的 MOF(sal-M-MOF,M = Fe,Co),它们是烯烃加氢的高活性固体催化剂。令人印象深刻的是,sal-Fe-MOF 表现出高达 145000 的非常高的周转数,并且已经回收和再使用了 15 多次。这项工作突出了开发基于 MOF 的丰富地球催化剂用于可持续化学合成的独特机会。