机构地区:[1]Materials Architecturing Research Center, Korea Institute of Science and Technology (KIST)),secul,Secrngbuk-gu,Republic of Korea [2]Department of Micro/Nano Systems, Korea University,Seoul,Seongbuk-gu,Republic of Korea [3]Computational Science Research Center, Korea Institute of Science and Technology (KIST),Secul,Secrngbuk-gu,Republic of Korea [4]Advanced Textile R&D Department, Korea Institute of Industrial Technology (KITECH),Amsan,Gyeonggi-do,Republic of Korea [5]Extreme Materials Research Center, Korea Institute of Science and Technology (KIST),Seoul,Seongbuk:gu,Repubic of Korea [6]Nanoscience and Technology, KIST School, University of Science and Technology,Seoul,Republic of Korea [7]Advanced Analysis and Data Center, Korea Institute of Science and Technology,Seoul,Seongbuk-gu,Republic of Korea [8]Display and Nanosensor Laboratory, School of Electrical Engineering, Korea University,Seoul,Seongbuk gu,Republic of Korea [9]KHU-KIST Department of Converging Science and Technology, Kyung Hee University,Seoul,Seongbuk-gu,Repubic of Korea
出 处:《Carbon Energy》2024年第11期234-255,共22页碳能源(英文)
基 金:This work was supported by the KIST Institutional Program(2E32461);the NationalResearch Council of Science&Technology(NST)grant(CPS21041-100);the National Research Foundation ofKorea(NRF)grant funded by the Korea Government(MSIT)(No.RS-2023-00209940,NRF-2022R 1F1A1068725, NRF-2022M3H4A7046278);Korea EnvironmentIndustry&Technology Institute(KEITI)through theEcological Imitation-based Environmental Pollution Man-agement Technology Development Project,funded by theKorea Ministry of Environment(MOE)(2021002800005).
摘 要:Atomically dispersed single-atom catalysts(SACs)on carbon supports show great promise for H_(2)O_(2) electrosynthesis,but conventional wet chemistry methods using particulate carbon blacks in powder form have limited their potential as two-electron(2^(e−))oxygen reduction reaction(ORR)catalysts.Here,we demonstrate high-performance Co SACs supported on a free-standing aligned carbon nanofiber(CNF)using electrospinning and arc plasma deposition(APD).Based on the surface oxidation treatment of aligned CNF and precise control of the deposition amount in a dry-based APD process,we successfully form densely populated Co SACs on aligned CNF.Through experimental analyses and density functional theory calculations,we reveal that Co SAC has a Co–N_(2)–O_(2) moiety with one epoxy group,leading to excellent 2^(e−)ORR activity.Furthermore,the aligned CNF significantly improves mass transfer in flow cells compared to randomly oriented CNF,showing an overpotential reduction of 30 mV and a 1.3-fold improvement(84.5%)in Faradaic efficiency,and finally achieves an outstanding production rate of 15.75 mol gcat^(−1) h^(−1) at 300 mA cm^(−2).The high-performance Co SAC supported on well-aligned CNF is also applied in an electro-Fenton process,demonstrating rapid removal of methylene blue and bisphenol F due to its exceptional 2e^(−)ORR activity.
关 键 词:arc plasma deposition ELECTRO-FENTON flow reactor hydrogen peroxide production oxygen reduction reaction single-atom catalysts
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