  It is a general challenge to design highly active or selective earth-abundant
metals for catalytic hydrogenation. Here, we demonstrated an effective
computational approach based on inverse molecular design theory to
deterministically search for optimal binding sites on Cu (100) surface through
the doping of Fe and/or Zn, and a stable Zn-doped Cu (100) surface was found
with minimal binding energy to H-atoms. We analyze the electronic structure
cause of the optimal binding sites using a new quantum chemistry method called
orbital-specific binding energy analysis. Compared to the 3d-orbitals of
surface Cu atoms, the 3d-orbitals of surface Zn-atoms show less binding energy
contribution and participation, and are much less influenced by the electronic
couplings of the media Cu atoms. Our study provides valuable green chemistry
insights on designing catalysts using earth-abundant metals, and may lead to
the development of novel Cu-based earth-abundant alloys for important catalytic
hydrogenation applications such as lignin degradation or CO2 transformation.
