posted on 2024-03-08, 20:38authored byWenhao Jing, Guiwei He, Shengjie Bai, Feng Wang, Ya Liu, Liejin Guo
For solar-driven overall pure water splitting, a superior
photocatalyst
with reasonable atomic and electronic structure is needed to be suitable
for both half-reactions, HER and OER. TiO2 has showcased
remarkable catalytic efficiency in the field of HER but it still encounters
obstacles in accomplishing proficient overall water splitting. Within
this work, following a sequential screening based on element type,
stability, electronic structure, and adsorption energy, we designed
a TiO2-based catalyst screening workflow for solar-driven
overall water splitting. This DFT-based workflow significantly reduced
both the time and trial-and-error costs associated with a traditional
experimental design. It precisely guided the synthesis of highly dispersed
Cu-loaded/N-doped TiO2, which facilitated sacrificial-agent-free
solar-driven overall water splitting, resulting in a solar to fuel
efficiency of 0.2% and an H2 yield of 1027.7 μmol/h/g.
Advanced DFT calculations revealed that the d–p orbital coupling
between Cu and N broke the scaling relationship of the O-based intermediates.
This work holds promise for extension to other catalytic reactions,
offering valuable insights into catalyst design endeavors.