摘要
Covalent organic frameworks(COFs)have been well developed in electrocatalytic systems owing to their controllable skeletons,porosities,and functions.However,the catalytic process in COFs remains underexplored,hindering an in-depth understanding of the catalytic mechanism.In this work,uniform Pt-N_(1)O_(1)Cl_(4)sites chelated via C-N and C=O bonds along the one-dimensional and open channels of TP-TTA-COF were established.Different from conventional single-metal sites constructed for the near-free platinum for hydrogen evolution,the as-constructed PtCl-COF showed 2e−oxygen reduction for H_(2)O_(2)production.We tracked the dynamic evolution process of atomic Pt sites in which Pt-N_(1)O_(1)Cl_(4)was transformed into Pt-N_(1)O_(1)(OH)_(2)using in situ X-ray adsorption.The theoretical calculations revealed that the strong Pt-support interaction in Pt-N_(1)O_(1)(OH)_(2)facilitated*OOH formation and thus led to higher selectivity and activity for the oxygen reduction reaction in the 2e−pathway.This work can expand the applications of COFs through the regulation of their local electronic states for the manipulation of the metal center.
出处
《SusMat》
2023年第3期379-389,共11页
可持续发展材料（英文）
基金
Natural Science Foundation of Shanghai,Grant/Award Number:20ZR1464000
CAS Project for Young Scientists in Basic Research,Grant/Award Number:YSBR-022。
