The purpose of this study is to develop novel P-Mo-V heteropoly compound catalysts for the oxidation of methacrolein to methacrylic acid.The introduction of Cu,as a modifying element,was employed to enhance the cataly...The purpose of this study is to develop novel P-Mo-V heteropoly compound catalysts for the oxidation of methacrolein to methacrylic acid.The introduction of Cu,as a modifying element,was employed to enhance the catalytic performance.Experimental results show that the addition of Cu significantly improved the catalyst performance,increasing the conversion rate of methacrolein from 17.2%to 84.2%,while the yield of methacrylic acid was boosted from 5.5%to 51.7%.A series of characterization results showed that both P-Mo-V and Cu-P-Mo-V catalysts primarily exhibited the crystal phase of[PMo_(12)O_(40)]^(3−),with a small amount of[PMo_(11)VO_(40)]^(3−)phase.However,the Cu-P-Mo-V catalyst exhibited much better oxidation–reduction ability compared to the P-Mo-V catalyst.Isolated Cu atoms were found to exist in a highly decentralized tetrahedral coordination structure,bridged by oxygen atoms within the heteropoly compound framework.The addition of Cu resulted in notable alterations in the modulation of the surface electronic structure,enhancement of oxidation–reduction ability,and optimization of the reaction pathway,thereby improving the overall catalytic activity of the catalyst.This study not only provides new insights into the modification of P-Mo-V heteropoly compound catalysts but also lays a foundation for understanding their catalytic mechanisms in organic synthesis reactions,demonstrating the potential of modifying elements in improving catalyst performance.展开更多
基金funding support received from China Petrochemical Corporation(Sinopec Group).
文摘The purpose of this study is to develop novel P-Mo-V heteropoly compound catalysts for the oxidation of methacrolein to methacrylic acid.The introduction of Cu,as a modifying element,was employed to enhance the catalytic performance.Experimental results show that the addition of Cu significantly improved the catalyst performance,increasing the conversion rate of methacrolein from 17.2%to 84.2%,while the yield of methacrylic acid was boosted from 5.5%to 51.7%.A series of characterization results showed that both P-Mo-V and Cu-P-Mo-V catalysts primarily exhibited the crystal phase of[PMo_(12)O_(40)]^(3−),with a small amount of[PMo_(11)VO_(40)]^(3−)phase.However,the Cu-P-Mo-V catalyst exhibited much better oxidation–reduction ability compared to the P-Mo-V catalyst.Isolated Cu atoms were found to exist in a highly decentralized tetrahedral coordination structure,bridged by oxygen atoms within the heteropoly compound framework.The addition of Cu resulted in notable alterations in the modulation of the surface electronic structure,enhancement of oxidation–reduction ability,and optimization of the reaction pathway,thereby improving the overall catalytic activity of the catalyst.This study not only provides new insights into the modification of P-Mo-V heteropoly compound catalysts but also lays a foundation for understanding their catalytic mechanisms in organic synthesis reactions,demonstrating the potential of modifying elements in improving catalyst performance.