The design of active acidic oxygen evolution reaction(OER)catalysts is of paramount importance to achieve efficient large-current-density industrial hydrogen fuel production via water electrolysis.Herein,we develop a ...The design of active acidic oxygen evolution reaction(OER)catalysts is of paramount importance to achieve efficient large-current-density industrial hydrogen fuel production via water electrolysis.Herein,we develop a Pt-based catalyst with high electrochemical activity for the OER in acidic conditions under a large current.We achieve this by modulating the electronic structure of Pt into a high-valence,electron-accessible Pt1^((2.4+δ)+)(δ=0-0.7)state during the reaction.This electron-accessible Pt1^((2.4+δ)+)single-site catalyst can effectively maintain a large OER current density of 120 mA cm^(-2)for more than 12 h in 0.5 M H_(2)SO_(4) at a low overpotential of 405 mV,and it shows a high mass activity of~3350 A gmetal^(-1)at 10 mA cm^(-2) current density and 232 mV overpotential.Using in situ synchrotron radiation infrared and X-ray absorption spectroscopies,we directly observe in an experiment that a key(*O)-Pt_(1)-C_(2)N_(2) intermediate is produced by the potential-driven structural optimization of square pyramidal Pt_(1)-C_(2)N_(2) moieties;this highly favors the dissociation of H_(2)O over Pt1^(2.4+δ)^(+)sites and prevents over-oxidation and dissolution of the active sites.展开更多
基金This work was supported by the National Natural Science Foundation of China(Grants No.12111530002,U1932212,U1932109,and 11875257)The reported study was also funded by RFBR(project number 21-52-53023).
文摘The design of active acidic oxygen evolution reaction(OER)catalysts is of paramount importance to achieve efficient large-current-density industrial hydrogen fuel production via water electrolysis.Herein,we develop a Pt-based catalyst with high electrochemical activity for the OER in acidic conditions under a large current.We achieve this by modulating the electronic structure of Pt into a high-valence,electron-accessible Pt1^((2.4+δ)+)(δ=0-0.7)state during the reaction.This electron-accessible Pt1^((2.4+δ)+)single-site catalyst can effectively maintain a large OER current density of 120 mA cm^(-2)for more than 12 h in 0.5 M H_(2)SO_(4) at a low overpotential of 405 mV,and it shows a high mass activity of~3350 A gmetal^(-1)at 10 mA cm^(-2) current density and 232 mV overpotential.Using in situ synchrotron radiation infrared and X-ray absorption spectroscopies,we directly observe in an experiment that a key(*O)-Pt_(1)-C_(2)N_(2) intermediate is produced by the potential-driven structural optimization of square pyramidal Pt_(1)-C_(2)N_(2) moieties;this highly favors the dissociation of H_(2)O over Pt1^(2.4+δ)^(+)sites and prevents over-oxidation and dissolution of the active sites.
