Bifunctional Promotion of Mg and Ga on Cu‐Based Hydrotalcite‐Derived Catalysts for CO ₂ Hydrogenation to Methanol

ABSTRACT CO 2 hydrogenation to high‐value methanol offers a promising pathway toward carbon neutrality and circular economy goals. However, improving the catalytic activity and long‐term stability of conventional Cu‐based catalysts is still challenging. Herein, we developed a series of hydrotalcite‐derived CuMgGa catalysts with varying Cu/Mg ratios and calcination temperatures. Systematic studies revealed that Mg provides abundant basic sites for CO 2 adsorption and stabilizes active Cu + species, while the unique layered structure of hydrotalcite precursors generates abundant Cu–MgGaO x interfaces, promotes oxygen vacancy formation and thus boosted catalytic performance. Furthermore, the robust interaction derived from hydrotalcite effectively suppressed Cu sintering and inhibited MgCO 3 formation, thus remarkably enhancing catalyst stability. The optimized 3CMG‐600 catalyst achieved a CO 2 conversion of 18.94% at 260°C, approaching thermodynamic equilibrium, and delivered a STY Cu of 521.19 mg CH3OH ·g Cu − 1 ·h −1 under 4 MPa and 14400 mL·g − 1 ·h −1 . Furthermore, the long‐term stability test of 270 h demonstrated that the hydrotalcite‐derived 3CMG‐600 catalyst exhibited superior resistance to Cu sintering compared to the 3CMG‐CP prepared by coprecipitation. This study offers mechanistic insights and a scalable materials strategy for advancing efficient and stable CO 2 ‐to‐methanol hydrogenation.