Theoretical explanation for the enhanced water-splitting catalytic activity in delithiated LiCoO$_2$

Layered LiCoO$_2$ (LCO) is important battery material not well know for its electrochemical catalytic activity. On the other hand, layered $3d$-metal-oxyhydroxides, including CoOOH, are very active water-splitting (oxygen-evolution reaction, OER) catalysts in alkaline media with structure very similar to LCO. In this work, we use DFT+U calculations to explain the enhancement effect in OER catalytic activity in the electrochemically delithiated LCO (De-LCO). We analyze the surface stability and OER activity of the 5 most stable surface facets of LCO and the De-LCO, with 50\% Li removed. Using standard thermodynamic approach of the theoretical OER overpotential, we show that all surface facets have more active sites under Li removal. Particularly, the non-polar facets are identified to be highly active and are further activated by the delithiation process, while the dominant (0001) surface has negligible activity. These findings are in very good agreement with our experimental investigation of LCO and De-LCO nanosheets and nanoparticles with well defined surface morphology.