The electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through the two-electron oxygen reduction reaction(2e-ORR)offers a promising alternative to the traditional anthraquinone process.However,this method often...The electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through the two-electron oxygen reduction reaction(2e-ORR)offers a promising alternative to the traditional anthraquinone process.However,this method often suffers from sluggish kinetics.In this study,we introduce a novel bismuth-doped cerium oxide(Bi-CeO_(2))composite,featuring hollow nanospheres and triangular nanoplate structures with highly dispersed Bi dopants on the CeO_(2) matrix.Notably,the morphology of Bi-CeO_(2) can be dynamically tuned between spheres and plates by adjusting the amounts of Bi dopants.This innovative 1%-Bi-CeO_(2) catalyst exhibits an exceptional H_(2)O_(2) selectivity of 62.3% and significantly enhanced H_(2)O_(2) yield,reaching 1.16 mol gcat^(−1) h^(−1) at 0.1 V with a high faradaic efficiency of 56.0%.Density functional theory(DFT)calculations reveal that Bi dopants effectively lower the free energy barrier for ^(*)OOH intermediate formation,thereby accelerating H_(2)O_(2) production.Additionally,when integrated into a dual-cathode system,1%-Bi-CeO_(2) demonstrates superior performance in removing organic dyes such as rhodamine B(RhB).This work offers a groundbreaking approach for designing high-efficiency heteroatom-doped catalysts for the 2e-ORR,paving the way for more effective electrochemical systems.展开更多
基金supported by the National Natural Science Foundation of China(No.22202114)the Natural Science Foundation of Shandong Province(No.ZR2022MB124 and ZR2022QB028)+1 种基金the China Postdoctoral Science Foundation(No.2021M701694)the Postdoctoral Science Foundation of Jiangsu Province(No.1006-YBA21038).
文摘The electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through the two-electron oxygen reduction reaction(2e-ORR)offers a promising alternative to the traditional anthraquinone process.However,this method often suffers from sluggish kinetics.In this study,we introduce a novel bismuth-doped cerium oxide(Bi-CeO_(2))composite,featuring hollow nanospheres and triangular nanoplate structures with highly dispersed Bi dopants on the CeO_(2) matrix.Notably,the morphology of Bi-CeO_(2) can be dynamically tuned between spheres and plates by adjusting the amounts of Bi dopants.This innovative 1%-Bi-CeO_(2) catalyst exhibits an exceptional H_(2)O_(2) selectivity of 62.3% and significantly enhanced H_(2)O_(2) yield,reaching 1.16 mol gcat^(−1) h^(−1) at 0.1 V with a high faradaic efficiency of 56.0%.Density functional theory(DFT)calculations reveal that Bi dopants effectively lower the free energy barrier for ^(*)OOH intermediate formation,thereby accelerating H_(2)O_(2) production.Additionally,when integrated into a dual-cathode system,1%-Bi-CeO_(2) demonstrates superior performance in removing organic dyes such as rhodamine B(RhB).This work offers a groundbreaking approach for designing high-efficiency heteroatom-doped catalysts for the 2e-ORR,paving the way for more effective electrochemical systems.
