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

Abstract

AbstractNi‐based catalysts have been widely studied in the hydrogenation of CO2 to CH4, but selective and efficient synthesis of higher alcohols (C2+OH) from CO2 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 C2+OH from CO2 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‐Ni3Zn1C0.7) by carburization of Zn‐incorporated Ni0, which can significantly enhance CO2 adsorption and the surface coverage of alkyl intermediates, and boost the C−C coupling to C2+OH rather than conventional CH4. This work opens a new catalytic avenue toward CO2 hydrogenation to C2+OH, and also provides an insightful example for the rational design of selective and efficient Ni‐based catalysts for CO2 hydrogenation to multiple carbon products.