Hollow-ZrO 2 @CuZnAl-LDH-Derived Catalyst for Direct CO 2 Hydrogenation to Methanol

Realizing net-zero emissions demands the design of innovative and efficient catalysts for CO2 valorization. Herein, we report a core@shell-structured catalyst precursor, h-ZrO2@Cu1.3ZnAl1.6-LDH, in which layered double hydroxide (LDH) platelets are arranged around hollow zirconia spheres (h-ZrO2), maximizing the interfacial area between the active LDH component and zirconia promoter. The h-ZrO2@Cu1.3ZnAl1.6-LDH-derived catalyst efficiently converts CO2 into methanol, reaching space-time yields (STYs) comparable to commercial catalysts, despite a 54% reduction in Cu loading (0.59 gMeOH gcat−1 h−1 at 250 °C, 45 bar, H2/CO2 = 3, 18,000 mL g−1 h−1 weight hourly space velocity, WHSV). Reporting the STY on a per gram copper basis highlights the efficiency of the catalyst: h-ZrO2@Cu1.3ZnAl1.6-LDH is twofold more active than the commercial catalyst under the same conditions (2.7 vs 1.3 gMeOH gcat−1 h−1).