Due to the weak nature of organic coordination bonds, metal-organic frameworks (MOFs) can hardly retain their intrinsic physicochemical properties and structural integrity when functioning in harsh heterogeneous reactions. Herein, a post-synthetic strategy to reinforce the MOF structure by inserting siliceous linkers inside is proposed, according to which a Si-infused UiO-66 (s-UiO-66) with well-developed porosity and exceptional thermal/structural stability is fabricated. This monodispersed Si-infused matrix with enlarged nanopores is then utilized as the catalyst host, and is highly conductive to confining ultrafine CuO nanoparticles with uniform dispersion. Targeting CO 2 hydrogenation to methanol reaction, the Cu-loaded s-UiO-66 (CuO/s-UiO-66) delivers a remarkable and efficient methanol production rate outperforming other Cu/ZrO 2 -based catalysts and the commercial catalyst. Moreover, the robust structure of CuO/s-UiO-66 prevents both copper phase and host material from aggregation during the catalyst preparation procedure and the reaction. In addition to material-oriented studies, in situ characterization techniques are employed to identify the active Cu component and key intermediates formed during the CO 2 hydrogenation reaction, separately. It is envisioned that this Si infusion strategy can be applied to construct stable host materials with boundary-defined structures from the pristine MOFs for broadened applications under extreme circumstances.
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