Hydrogen peroxide(H2O2)is a very useful chemical reagent,but the current industrial methods for its production suffer from serious energy consumption problems.Using high-activity and high-selectivity catalysts to elec...Hydrogen peroxide(H2O2)is a very useful chemical reagent,but the current industrial methods for its production suffer from serious energy consumption problems.Using high-activity and high-selectivity catalysts to electrocatalyze the oxygen reduction reaction(ORR)through a two-electron(2e^-)pathway is a very promising route to produce H2O2.In this work,we obtained partially oxidized multi-walled carbon nanotubes(MWCNTs)with controlled structure and composition by oxidation with concentrated sulfate and potassium permanganate at 40℃ for 1 h(O-CNTs-40-1).The outer layers of O-CNTs-40-1 are damaged with defects and oxygen-containing functional groups,while the inner layers are maintained intact.The optimized structure and composition of the partially oxidized MWCNTs ensure that O-CNTs-40-1 possesses both a sufficient number of catalytic sites and good conductivity.The results of rotating ring disk electrode measurements reveal that,among all oxidized MWCNTs,O-CNTs-40-1 shows the greatest improvement in hydrogen peroxide selectivity(from ~ 30% to ~ 50%)and electron transfer number(from ~ 3.4 to ~ 3.0)compared to those of the raw MWCNTs.The results of electrochemical impedance spectroscopy measurements indicate that both the charge-transfer and intrinsic resistances of O-CNTs-40-1 are lower than those of the raw MWCNTs and of the other oxidized MWCNTs.Finally,direct tests of the H2O2 production confirm the greatly improved catalytic activity of O-CNTs-40-1 relative to that of the raw MWCNTs.展开更多
基金supported by the National Natural Science Foundation of China(21576299,21576300)Guangzhou Science and Technology Project(201607010104,201707010079)+3 种基金Science and Technology Planning Project of Guangdong Province(2017A050501009)the National Key Research and Development Program of China(2016YFB0101204)Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program(2016TQ03N322)the fundamental Research Funds for Central Universities(17lgzd14)~~
文摘Hydrogen peroxide(H2O2)is a very useful chemical reagent,but the current industrial methods for its production suffer from serious energy consumption problems.Using high-activity and high-selectivity catalysts to electrocatalyze the oxygen reduction reaction(ORR)through a two-electron(2e^-)pathway is a very promising route to produce H2O2.In this work,we obtained partially oxidized multi-walled carbon nanotubes(MWCNTs)with controlled structure and composition by oxidation with concentrated sulfate and potassium permanganate at 40℃ for 1 h(O-CNTs-40-1).The outer layers of O-CNTs-40-1 are damaged with defects and oxygen-containing functional groups,while the inner layers are maintained intact.The optimized structure and composition of the partially oxidized MWCNTs ensure that O-CNTs-40-1 possesses both a sufficient number of catalytic sites and good conductivity.The results of rotating ring disk electrode measurements reveal that,among all oxidized MWCNTs,O-CNTs-40-1 shows the greatest improvement in hydrogen peroxide selectivity(from ~ 30% to ~ 50%)and electron transfer number(from ~ 3.4 to ~ 3.0)compared to those of the raw MWCNTs.The results of electrochemical impedance spectroscopy measurements indicate that both the charge-transfer and intrinsic resistances of O-CNTs-40-1 are lower than those of the raw MWCNTs and of the other oxidized MWCNTs.Finally,direct tests of the H2O2 production confirm the greatly improved catalytic activity of O-CNTs-40-1 relative to that of the raw MWCNTs.
