https://scholars.lib.ntu.edu.tw/handle/123456789/626236
標題: | Construction of N, P Co-Doped Carbon Frames Anchored with Fe Single Atoms and Fe2P Nanoparticles as a Robust Coupling Catalyst for Electrocatalytic Oxygen Reduction | 作者: | Pan Y Ma X Wang M Yang X Liu S Chen H.-C Zhuang Z Zhang Y Cheong W.-C Zhang C Cao X Shen R Xu Q Zhu W Liu Y Wang X Zhang X Yan W Li J HAO MING CHEN Chen C Li Y. |
關鍵字: | coupling catalysts; electrocatalysis; oxygen reduction reaction; single-atom catalysts | 公開日期: | 2022 | 來源出版物: | Advanced Materials | 摘要: | A coupling catalyst of highly dispersed N, P co-doped carbon frames (NPCFs) anchored with Fe single atoms (SAs) and Fe2P nanoparticles (NPs) is synthesized by a novel in situ doping–adsorption–phosphatization strategy for the electrocatalytic oxygen reduction reaction (ORR). The optimized Fe SAs-Fe2P NPs/NPCFs-2.5 catalyst shows a superior ORR activity and stability in 0.5 m H2SO4 and 0.1 m KOH, respectively. Theoretical calculations reveal a synergistic effect, in that the existence of Fe2P weakens the adsorption of ORR intermediates on active sites and lowers the reaction free energy. The doped P atoms with a strong electron-donating ability elevate the energy level of Fe-3d orbitals and facilitate the adsorption of O2. The active Fe atoms exist in a low oxidation state and are less positively charged, and they serve as an electron reservoir capable of donating and releasing electrons, thus improving the ORR activity. Operando and in situ characterization results indicate that the atomically dispersed Fe-N4/Fe-P coupled active centers in the Fe SAs-Fe2P NPs/NPCFs-2.5 catalyst are characteristic of the different catalytic mechanisms in acidic and alkaline media. This work proposes a novel idea for constructing coupling catalysts with atomic-level precision and provides a strong reference for the development of high-efficiency ORR electrocatalysts for practical application. © 2022 Wiley-VCH GmbH. |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85131962371&doi=10.1002%2fadma.202203621&partnerID=40&md5=8ab206206d7557f6c265ec30c74f7e65 https://scholars.lib.ntu.edu.tw/handle/123456789/626236 |
ISSN: | 09359648 | DOI: | 10.1002/adma.202203621 | SDG/關鍵字: | Adsorption; Atoms; Carbon; Electrocatalysis; Electrolytic reduction; Free energy; Iron; Iron compounds; Nanocatalysts; Nanoparticles; Oxygen; Potassium hydroxide; Reaction intermediates; Synthesis (chemical); Co-doped; Coupling catalyst; Doped carbons; Electrocatalytic oxygen reduction; Oxygen reduction reaction; Reaction activity; Single-atom catalyst; Single-atoms; ]+ catalyst; Electrocatalysts |
顯示於: | 化學系 |
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