Molecular interactions with both oxides and metals are essential for heterogenous catalysis, leading to remarkable synergistic impacts on activity and selectivity. Here, we show that the direct link between the two phases (and not merely being together) is required to selectively hydrogenate CO2 to methanol on catalysts containing Cu and ZrO2. Materials consisting of isolated Cu particles or atomically dispersed Cu–O–Zr sites only catalyze the reverse water-gas shift reaction. In contrast, a metal organic framework structure (UiO-66) with Cu nanoparticles occupying missing-linker defects maximizes the fraction of metallic Cu interfaced to ZrO2 nodes leading to a material with high adsorption capacity for CO2 and high activity and selectivity for low-temperature methanol synthesis.
Bibliographical noteFunding Information:
We gratefully acknowledge support for this work from the Inorganometallic Catalyst Design Center, an EFRC funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (DE-SC0012702). Y.Z., L.K., D.M.C., J.F., and O. Y.G. acknowledge support from the DOE Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences (Transdisciplinary Approaches to Realize Novel Catalytic Pathways to Energy Carriers, FWP 47319). Portions of this work were performed at the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory, and was supported by DOE (under Contract No. DE-AC02-06CH11357) and the Canadian Light Source and its funding partners. X-ray adsorption spectra were taken with the help of Dr. Mahalingam Balasubramanian.
© 2020, The Author(s).