Engineering Catalysis within a Saturated In(III)-Based MOF Possessing Dynamic Ligand–Metal Bonding

Citations Over TimeTop 10% of 2022 papers

Abstract

Metal-organic frameworks have developed into a formidable heterogeneous catalysis platform in recent years. It is well established that thermolysis of coordinated solvents from MOF nodes can render highly reactive, coordinatively unsaturated metal complexes which are stabilized via site isolation and serve as active sites in catalysis. Such approaches are limited to frameworks featuring solvated transition-metal complexes and must be stable toward the formation of "permanent" open metal sites. Herein, we exploit the hemilability of metal-carboxylate bonds to generate transient open metal sites in an In(III) MOF, pertinent to In-centered catalysis. The transient open metal sites catalyze the Strecker reaction over multiple cycles without loss of activity or crystallinity. We employ computational and spectroscopic methods to confirm the formation of open metal sites via transient dissociation of In(III)-carboxylate bonds. Furthermore, the amount of transient open metal sites within the material and thus the catalytic performance can be temperature-modulated.

Related Papers

• → Enhanced catalytic activity of Pt/Al2O3 on the CH4 SCR(2011)24 cited
• → Catalytic performance of Ni/γ-Al2O3 for hydrogenation of 2-ethyl-2-hexenal(2017)15 cited
• → Catalytic reduction of N2O with CH4 over FeAlPO-5 catalyst(2008)15 cited
• → Determining influence of catalyst-reductant morphology on two different mechanisms of SCR by MOFs(2021)3 cited
• → Catalytic activity of H3PMo12−XWXO40 and H6P2MO18−XWXO62 heteropolyacid (HPA) catalysis in the direct preparation of dichloropropanol (DCP) from glycerol(2008)9 cited