Catalytic tandem synthesis of fine chemicals using the in situ-formed intermediates by electrocatalytic reactions has increasingly attracted attention in recent years.The difficulty lies in the low local concentration...Catalytic tandem synthesis of fine chemicals using the in situ-formed intermediates by electrocatalytic reactions has increasingly attracted attention in recent years.The difficulty lies in the low local concentration of intermediates because of the slow formation rates in the catalytically electrochemical process.We showcase an efficient tandem epoxidation of propene,which is accelerated by the in situ-generated hydrogen peroxide(H_(2)O_(2)).The catalysts of iron-doped tubular mesoporous carbons feature ultrathin carbon walls and record-high exposed external surface areas,which enable a H_(2)O_(2) formation rate of 747.7 mmol gcat^(-1) h^(-1) at 0.4 V versus reversible hydrogen electrode,together with a H_(2)O_(2) Faradaic efficiency of nearly 100%.A positive correlation between the exposed external surface area and the oxygen reduction activity is experimentally observed.By utilizing the in situ-generated H_(2)O_(2),the tandem epoxidation of propylene displays a yield rate of 80.3μmol gTS-1^(-1) h^(-1) for propylene oxide.The high performance originates from the high local concentration of H_(2)O_(2) surrounding the titanium silicalite-1 catalysts for propylene epoxidation.The results may inspire other tandem electrochemical reactions by using the mesoporous catalysts for synthesis of building block chemicals.展开更多
基金supported by the National Natural Science Foundation of China(grant nos.22275027 and 21975037)the Fundamental Research Funds for the Central Universities(grant nos.DUT22QN206 and DUT22LAB607).
文摘Catalytic tandem synthesis of fine chemicals using the in situ-formed intermediates by electrocatalytic reactions has increasingly attracted attention in recent years.The difficulty lies in the low local concentration of intermediates because of the slow formation rates in the catalytically electrochemical process.We showcase an efficient tandem epoxidation of propene,which is accelerated by the in situ-generated hydrogen peroxide(H_(2)O_(2)).The catalysts of iron-doped tubular mesoporous carbons feature ultrathin carbon walls and record-high exposed external surface areas,which enable a H_(2)O_(2) formation rate of 747.7 mmol gcat^(-1) h^(-1) at 0.4 V versus reversible hydrogen electrode,together with a H_(2)O_(2) Faradaic efficiency of nearly 100%.A positive correlation between the exposed external surface area and the oxygen reduction activity is experimentally observed.By utilizing the in situ-generated H_(2)O_(2),the tandem epoxidation of propylene displays a yield rate of 80.3μmol gTS-1^(-1) h^(-1) for propylene oxide.The high performance originates from the high local concentration of H_(2)O_(2) surrounding the titanium silicalite-1 catalysts for propylene epoxidation.The results may inspire other tandem electrochemical reactions by using the mesoporous catalysts for synthesis of building block chemicals.
