Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
It is reported for the first time that the Pt - Ru/C catalyst was prepared with the solid phase reaction method.Cyclic voltammetric measurements indicated that the anodic peak potential of ethanol at the electrode wit...It is reported for the first time that the Pt - Ru/C catalyst was prepared with the solid phase reaction method.Cyclic voltammetric measurements indicated that the anodic peak potential of ethanol at the electrode with the Pt - Ru/C catalyst prepared with the solid phase reaction method was0.54V and the peak current was100mA · cm -2 .While the anodic peak potential and peak current were0.64V and43mA · cm -2 respectively at the Pt - Ru/C catalyst prepared with the traditional liquid phase reaction method.It illustrated that the electrocatalytic activity of the Pt - Ru/C catalyst prepared with the solid phase reaction method was much better than that of the Pt - Ru/C catalyst prepared with the traditional liquid phase reaction method.It is because the Pt - Ru/C catalyst prepared with the solid phase reaction method is of low crystallinity and high dispersivity.展开更多
基金supported by the National Key R&D Program of China(2021YFA1502802)the National Natural Science Foundation of China(U21B2092,22202213,22402210,22502215,22502214,22572200,and 22579171)+4 种基金the International Partnership Program of Chinese Academy of Sciences(172GJHZ2022028MI)the Shenyang Bureau of Science and Technology(24-213-3-25)the Natural Science Foundation of Liaoning Province(2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119The XAS experiments were conducted in Beijing Synchrotron Radiation Facility(BSRF)and Shanghai Synchrotron Radiation Facility(SSRF).
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
文摘It is reported for the first time that the Pt - Ru/C catalyst was prepared with the solid phase reaction method.Cyclic voltammetric measurements indicated that the anodic peak potential of ethanol at the electrode with the Pt - Ru/C catalyst prepared with the solid phase reaction method was0.54V and the peak current was100mA · cm -2 .While the anodic peak potential and peak current were0.64V and43mA · cm -2 respectively at the Pt - Ru/C catalyst prepared with the traditional liquid phase reaction method.It illustrated that the electrocatalytic activity of the Pt - Ru/C catalyst prepared with the solid phase reaction method was much better than that of the Pt - Ru/C catalyst prepared with the traditional liquid phase reaction method.It is because the Pt - Ru/C catalyst prepared with the solid phase reaction method is of low crystallinity and high dispersivity.
