Optimizing Binding Energies of Key Intermediates for CO 2 Hydrogenation to Methanol over Oxide-Supported Copper

Rational optimization of catalytic performance has been one of the major challenges in catalysis. Here we report a bottom-up study on the ability of TiO2 and ZrO2 to optimize the CO2 conversion to methanol on Cu, using combined density functional theory (DFT) calculations, kinetic Monte Carlo (KMC) simulations, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements, and steady-state flow reactor tests. The theoretical results from DFT and KMC agree with in situ DRIFTS measurements, showing that both TiO2 and ZrO2 help to promote methanol synthesis on Cu via carboxyl intermediates and the reverse water-gas-shift (RWGS) pathway; the formate intermediates, on the other hand,…

• UD
  U.S. Department of Energy

  Awards: -AC02-05CH11231, AC05-00OR22725, 05CH11231, AC02-05CH11231, SC0012704, DE-AC02, DE-AC02-05CH11231, DE-AC05, 00OR22725, DE-AC02-
• NE
  National Energy Research Scientific Computing Center

  Awards: 05CH11231, AC02-05CH11231, DE-AC05-00OR22725
• OO
  Office of Science

  Awards: DE-AC05-00OR22725, AC02-05CH11231, -AC02-05CH11231, DE-AC02, SC0012704, AC05-00OR22725, DE-SC0012704
• OR
  Oak Ridge National Laboratory

  Awards: AC05-00OR22725, DE-AC02-05CH11231
• BN
  Brookhaven National Laboratory

  Awards: SC0012704, DE-AC02-05CH11231