Charge transfer between molecules and catalysts plays a critical role in determining the efficiency and yield of photo-chemical catalytic processes. In this paper, we study light-induced electron transfer between transition metal doped aluminium clusters and CO2 molecules using first-principles time-dependent density-functional theory. Specifically, we carry out calculations for a range of dopants (Zr, Mn, Fe, Ru, Co, Ni and Cu) and find that the resulting systems fall into two categories: Cu- and Fe-doped clusters exhibit no ground state charge transfer, weak CO2 adsorption and light-induced electron transfer into the CO2. In all other systems, we observe ground state electron transfer into the CO2 resulting in strong adsorption and predominantly light-induced electron back-transfer from the CO2 into the cluster. These findings pave the way towards a rational design of atomically precise aluminium photo-catalysts.
@article{arxiv.2103.14405,
title = {Light Induced Charge Transfer from Transition-metal Doped Aluminium Clusters to Carbon Dioxide},
author = {Alexandra Göbel and Angel Rubio and Johannes Lischner},
journal= {arXiv preprint arXiv:2103.14405},
year = {2021}
}