The development of active water oxidation catalysts for water splitting has stimulated considerable interest.Herein,the design and building of single atom Co sites using a supramolecular tailoring strategy are reporte...The development of active water oxidation catalysts for water splitting has stimulated considerable interest.Herein,the design and building of single atom Co sites using a supramolecular tailoring strategy are reported,that is,the introduction of pillar[4]arene[1]quinone(P4A1Q)permits mononuclear Co species stereoelectronically assembled on MoS_(2)matrix to construct an atomically dispersed MoS_(2)@Co catalyst with modulated local electronic structure,definite chemical environment and enhanced oxygen evolution reaction performance.Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygen-containing intermediates,endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity,with a low overpotential of 370 mV at 10 mA cm^(-2)and a small Tafel slope of 90 mV dec^(-1).The extendable potential of this strategy to other electrocatalysts such as MoS_(2)@Ni and MoS_(2)@Zn,and other applications such as the hydrogen evolution reaction was also demonstrated.This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.展开更多
基金the financial support from the“Young Talent Support Plan”(no.050700-71240000000046)of Xi’an Jiaotong Universitythe Natural Science Foundation of Shaanxi Province(no.2021JM-006)+3 种基金the“Young Talent Start-up Fund”Project of Zhengzhou University(no.32212778)the Joint Project from the Henan Provincial and the China National Natural Science Foundations(no.U2004208)the Ministry of Education Singapore under its Academic Research Funds(no.RG3/21,RG2/22,and RG85/22)the Agency for Science,Technology and Research(A*STAR)Singapore through its Manufacturing,Trade and Connectivity(MTC)Individual Research Grant(no.M21K2c0105)
文摘The development of active water oxidation catalysts for water splitting has stimulated considerable interest.Herein,the design and building of single atom Co sites using a supramolecular tailoring strategy are reported,that is,the introduction of pillar[4]arene[1]quinone(P4A1Q)permits mononuclear Co species stereoelectronically assembled on MoS_(2)matrix to construct an atomically dispersed MoS_(2)@Co catalyst with modulated local electronic structure,definite chemical environment and enhanced oxygen evolution reaction performance.Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygen-containing intermediates,endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity,with a low overpotential of 370 mV at 10 mA cm^(-2)and a small Tafel slope of 90 mV dec^(-1).The extendable potential of this strategy to other electrocatalysts such as MoS_(2)@Ni and MoS_(2)@Zn,and other applications such as the hydrogen evolution reaction was also demonstrated.This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.
