A high-performance core-sheath C@CuSiO3 nanocatalyst for CO2 hydrogenation to methanol achieved by Cu-C interaction

Catalytic hydrogenation of CO₂ to chemicals and alternative fuels such as methanol is an attractive approach for CO₂ utilization and hydrogen storage. Copper silicate is considered as efficient for hydrogenation of C-O/C=O bonds due to the synergistic effect from its unique dual-sites of Cu⁰-Cu⁺. However, it still confronts great obstacles of poor CO₂ conversion and methanol selectivity. Herein, we introduce carbon nanotubes (CNTs) to electronically interact with Cu⁰-Cu⁺ sites, achieving CO₂ conversion of ∼ 25 % with methanol selectivity up to 80 %, which breaks the equilibrium selectivity (∼51 %) on this condition. Intrinsically, CNTs could not alter the *HOCO and *CO intermediates pathway of hydrogenation over Cu⁰-Cu⁺ sites, but accelerate H₂ dissociation on Cu^δ+ (0 < δ < 1) originated from Cu⁰-C interaction at their interface. This leads to a local concentration enrichment of active H to boost deep hydrogenation to methanol. These findings open a new avenue for designing highly efficient and selective catalytic hydrogenation systems.