The discovery of new materials for efficient transformation of carbon dioxide (CO2) into desired fuel can revolutionize large-scale renewable energy storage and mitigate environmental damage due to carbon emissions. In this work, we discovered an operando generated stable Ni-In kinetic phase that selectively converts CO2 to methanol (CTM) at low pressure compared to the state-of-the-art materials. The catalytic nature of a well-known methanation catalyst, nickel, has been tuned with the introduction of inactive indium, which enhances the CTM process. The remarkable change in the mechanistic pathways toward methanol production has been mapped by operando diffuse reflectance infrared Fourier transform spectroscopy analysis, corroborated by first-principles calculations. The ordered arrangement and pronounced electronegativity difference between metals are attributed to the complete shift in mechanism. The approach and findings of this work provide a unique advance toward the next-generation catalyst discovery for going beyond the state-of-the-art in CO2 reduction technologies.

Foreign