In‐Situ‐Formed Potassium‐Modified Nickel‐Zinc Carbide Boosts Production of Higher Alcohols beyond CH4 in CO2 Hydrogenation

Abstract Ni‐based catalysts have been widely studied in the hydrogenation of CO 2 to CH 4 , but selective and efficient synthesis of higher alcohols (C 2+ OH) from CO 2 hydrogenation over Ni‐based catalyst is still challenging due to successive hydrogenation of C1 intermediates leading to methanation. Herein, we report an unprecedented synthesis of C 2+ OH from CO 2 hydrogenation over K‐modified Ni−Zn bimetal catalyst with promising activity and selectivity. Systematic experiments (including XRD, in situ spectroscopic characterization) and computational studies reveal the in situ generation of an active K‐modified Ni−Zn carbide (K‐Ni 3 Zn 1 C 0.7 ) by carburization of Zn‐incorporated Ni 0 , which can significantly enhance CO 2 adsorption and the surface coverage of alkyl intermediates, and boost the C−C coupling to C 2+ OH rather than conventional CH 4 . This work opens a new catalytic avenue toward CO 2 hydrogenation to C 2+ OH, and also provides an insightful example for the rational design of selective and efficient Ni‐based catalysts for CO 2 hydrogenation to multiple carbon products.