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Capsule-structured copper-zinc catalyst for highly efficient hydrogenation of carbon dioxide to methanol.

To develop a new and efficient CO2-to-methanol catalyst is of extreme significance, but still remains a challenge. Herein we report an innovative indirect two-step improvement strategy to synthesize a highly efficient capsule-structured copper-based CO2-to-methanol catalyst (CZA-r@CZM). It consists of a structurally reconstructed millimeter-sized Cu/ZnO/Al2O3 core (CZA-r) with intensified Cu-ZnO interaction via a facile hydrothermal treatment in an alkaline aqueous solution and a Cu/ZnO/MgO (CZM) shell prepared by an ethylene glycol-assisted physically coating method, in which the CZA-r core displays 2.7 times higher CO2 hydrogenation activity with 2.0 times higher CO selectivity than the previously reported Cu/ZnO/Al2O3 (CZA-p), while the CZM shell can efficiently catalyze hydrogenation of the as-formed CO over CZA-r core to methanol as it passes the shell. As a result, the developed capsule-structured CZA-r@CZM catalyst exhibits 2.4 times higher CO2 conversion with the 1.8 times higher turnover frequency and 2.3 folds higher methanol space-time yield than the CZA-p catalyst (729.8 vs 312.6 gMeOH kgcat-1 h-1). In situ DRIFTs experiments reveal that the CO2 hydrogenation reaction proceeds through a reverse water gas shift followed by CO-hydrogenation pathway via *H3CO intermediate. This work not only produces a novel and efficient CO2-to-methanol catalyst, but also opens a new avenue for designing much superior catalysts for the other consecutive transformations.