Highly Selective Conversion of Carbon Dioxide to Methanol through a Cu−ZnO−Al2O3−ZrO2/Cu−MOR Tandem Catalyst

Abstract Methanol formation from CO 2 hydrogenation attracts great attention in view of utilization of carbon resources. However, CO 2 transformation to methanol is challenging because of the thermodynamic equilibrium restriction and water‐caused catalyst deactivation. It is desired, therefore, to develop highly active, selective and stable catalysts for CO 2 hydrogenation to methanol. Herein, we propose a novel tandem catalyst composed of Cu−ZnO−Al 2 O 3 −ZrO 2 (CZAZ) and Cu−MOR for highly selective conversion of CO 2 to methanol. During CO 2 hydrogenation by the CZAZ catalyst, the by‐product methane is continuously transformed to methanol through reaction with water via the Cu−MOR catalyst, thus enhancing CO 2 conversion and methanol selectivity. Under mild reaction conditions (200 °C and 3.0 MPa), high CO 2 conversion (40.7 %) and methanol selectivity (97.6 %) are achieved, outperforming state‐of‐the‐art CO 2 hydrogenation catalysts. Further, water‐caused deactivation of the catalyst through aggregation and densification is suppressed owing to water consumption via methane oxidation to methanol, validating a high CZAZ/Cu−MOR tandem catalyst stability.