Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis ...Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC(Pt_(1)/MoC)by using facile and controllable arc-discharge strategy under extreme conditions.The high temperature(up to 4000℃)provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions.The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation.The initial turnover frequency of 3710 h^(-1)is greater than those of previously reported samples by an order of magnitude under 2 MPa H_(2)at 100℃.The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C,C=N,and C=O.The facile,one-step,and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.展开更多
基金This work was financially supported by the National Key Research and Development Program of China(2016YFB0901600)the NSF of China(21872166)the Key Research Program of Chinese Academy of Sciences(QYZDJ-SSW-JSC013 and KGZD-EW-T06).
文摘Although single-atom catalysts significantly improve the atom utilization efficiency,the multistep preparation procedures are complicated and difficult to control.Herein,we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC(Pt_(1)/MoC)by using facile and controllable arc-discharge strategy under extreme conditions.The high temperature(up to 4000℃)provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions.The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation.The initial turnover frequency of 3710 h^(-1)is greater than those of previously reported samples by an order of magnitude under 2 MPa H_(2)at 100℃.The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C,C=N,and C=O.The facile,one-step,and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.
