Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing hi...Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing highly active,selective and cost-effective electrocatalysts.The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification.We herein report a phosphorus and selenium tuning Co-based non-precious catalyst(CoPSe)toward two-electron oxygen reduction reaction(2e–ORR)to produce H2O2 in acidic media.The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP.The results demonstrated that the CoPSe catalyst exhibited the optimized 2e–ORR activity compared with CoP and CoSe.It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85%in a wide potential range(0–0.5 V).Notably,the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transitionmetal based 2e–ORR catalysts.Finally,combining with electro-Fenton reaction,an on-site system was constructed for efficient degradation of organic pollutants.This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media.展开更多
Electrocatalytic production of hydrogen peroxide(H_(2)O_(2))by two-electron oxygen reduction reaction(2e^(-)ORR)under acidic condition has been considered to have great application value.Co nanoparticles(CoNPs)coupled...Electrocatalytic production of hydrogen peroxide(H_(2)O_(2))by two-electron oxygen reduction reaction(2e^(-)ORR)under acidic condition has been considered to have great application value.Co nanoparticles(CoNPs)coupled with N-doped carbon are a class of potential electrocatalysts.The effective strategies to further enhance their performances are to improve the active sites and stability.Herein,the material containing ultrafine CoNPs confined in a nitrogen-doped carbon matrix(NC@CoNPs)was synthesized by pyrolyzing corresponding precursors,which was obtained through regulating the topological structure of ZIF-67/ZIF-8 with dopamine(DA).The DA self-polymerization process induced the formation of CoNPs with smaller sizes and formed polydopamine film decreased the detachment of CoNPs from the catalyst.High density of Co-N_(x) active sites and defective sites could be identified on NC@CoNPs,leading to high activity and H_(2)O_(2) selectivity,with an onset potential of 0.57 V(vs.RHE)and∼90%selectivity in a wide potential range.An on-site electrochemical removal of organic pollutant was achieved rapidly through an electro-Fenton process,demonstrating its great promise for on-site water treatment application.展开更多
基金the National Natural Science Foundation of China(Nos.21805052,21974031,2278092)Science and Technology Research Project of Guangzhou(Nos.202102020787 and 202201000002)+2 种基金Department of Science&Technology of Guangdong Province(No.2022A156)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.20225546)the Innovation&Entrepreneurship for the College Students of Guangzhou University(No.XJ202111078175).
文摘Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing highly active,selective and cost-effective electrocatalysts.The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification.We herein report a phosphorus and selenium tuning Co-based non-precious catalyst(CoPSe)toward two-electron oxygen reduction reaction(2e–ORR)to produce H2O2 in acidic media.The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP.The results demonstrated that the CoPSe catalyst exhibited the optimized 2e–ORR activity compared with CoP and CoSe.It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85%in a wide potential range(0–0.5 V).Notably,the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transitionmetal based 2e–ORR catalysts.Finally,combining with electro-Fenton reaction,an on-site system was constructed for efficient degradation of organic pollutants.This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media.
基金financial support from the Natural Science Foundation of China(Nos.21805052 and 2278092)Science and Technology Research Project of Guangzhou(Nos.202102020787 and 202201000002)+1 种基金Department of Science&Technology of Guangdong Province(ID:2022A156),Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.20225546)the Innovation&Entrepreneurship for the College Students of Guangzhou University(No.XJ202111078175).
文摘Electrocatalytic production of hydrogen peroxide(H_(2)O_(2))by two-electron oxygen reduction reaction(2e^(-)ORR)under acidic condition has been considered to have great application value.Co nanoparticles(CoNPs)coupled with N-doped carbon are a class of potential electrocatalysts.The effective strategies to further enhance their performances are to improve the active sites and stability.Herein,the material containing ultrafine CoNPs confined in a nitrogen-doped carbon matrix(NC@CoNPs)was synthesized by pyrolyzing corresponding precursors,which was obtained through regulating the topological structure of ZIF-67/ZIF-8 with dopamine(DA).The DA self-polymerization process induced the formation of CoNPs with smaller sizes and formed polydopamine film decreased the detachment of CoNPs from the catalyst.High density of Co-N_(x) active sites and defective sites could be identified on NC@CoNPs,leading to high activity and H_(2)O_(2) selectivity,with an onset potential of 0.57 V(vs.RHE)and∼90%selectivity in a wide potential range.An on-site electrochemical removal of organic pollutant was achieved rapidly through an electro-Fenton process,demonstrating its great promise for on-site water treatment application.