Molecule functionalization to facilitate electrocatalytic oxygen reduction on graphdiyne

Chemical doping is verified to be a promising strategy to regulate local electron distribution and further promote the poor intrinsic catalytic activity of graphdiyne. However, the current doping approach still faces problems such as precise doping for creating active sites and the destruction of graphdiyne skeleton calling for high temperature. Here, we achieved charge redistribution on graphdiyne surface through molecule functionalization. A p-type molecule-F4TCNQ (2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodime thane) was introduced and the site-defined functionalization was accomplished. Theoretical calculations showed that the charge transfer ability is improved and graphdiyne becomes positively charged. The oxygen reduction electrocatalysis was conducted as a proof of principle, where the electronic states of sp hybridized C active site was tuned toward favorable reaction intermediates' adsorption. Such work from both theoretical prediction and experimental validation, found that molecule functionalization is effective to promote the electrocatalytic oxygen reduction, which creates new possibilities for graphdiyne's applications in different electrochemical reactions. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

Automated summary

Chemical doping is a promising strategy to enhance the catalytic activity of graphdiyne, with molecule functionalization showing potential in promoting electrocatalytic oxygen reduction reactions.