TY - JOUR
T1 - Promoting oxygen reduction kinetics of single Fe sites for robust neutral Zn-air batteries via engineering synergistic Fe nanocluster as proton-feeding center
AU - Xu, Ren
AU - Wang, Xingkun
AU - Sun, Mingzi
AU - Zhang, Canhui
AU - Li, Cheng
AU - Cao, Zhengwen
AU - Gu, Meng
AU - Huang, Bolong
AU - Huang, Minghua
PY - 2023/11/1
Y1 - 2023/11/1
N2 - Constructing highly efficient and cost-effective catalysts for neutral oxygen reduction reaction (ORR) remains extremely challenging due to the sluggish reaction kinetics resulting from the low ionic conductivity and limited OH− concentration in the neutral electrolytes. Herein, we intentionally integrate the atomic Fe-N4 sites and Fe nanoclusters on N-doped multimodally porous carbon (FeSA+NC@NMPC) to achieve coherent optimization of rapid oxygen-containing intermediate conversions and fast water dissociation to provide abundant protons for boosting neutral ORR performance. As expected, the FeSA+NC@NMPC exhibits an excellent half-wave potential of 0.76 V in 0.1 M phosphate buffer solutions, outperforming that of commercial Pt/C (0.73 V). Theoretical calculations reveal the synergistic effect between atomic Fe-N4 sites and Fe nanoclusters, in which the former possess stable O2 adsorption and rapid intermediate conversion, while the latter facilitates fast water dissociation to supply protons for accelerating the proton-coupled electron transfer process. Moreover, the FeSA+NC@NMPC-based neutral zinc-air batteries afford a high open-circuit potential of 1.42 V and outstanding cycling stability at 5 mA cm−2 for 100 h. This work utilizes the advantages of both single sites and clusters of Fe to provide an in-depth understanding of the neutral ORR mechanism and advances the development of related energy storage and conversion technologies. © 2023 Elsevier B.V.
AB - Constructing highly efficient and cost-effective catalysts for neutral oxygen reduction reaction (ORR) remains extremely challenging due to the sluggish reaction kinetics resulting from the low ionic conductivity and limited OH− concentration in the neutral electrolytes. Herein, we intentionally integrate the atomic Fe-N4 sites and Fe nanoclusters on N-doped multimodally porous carbon (FeSA+NC@NMPC) to achieve coherent optimization of rapid oxygen-containing intermediate conversions and fast water dissociation to provide abundant protons for boosting neutral ORR performance. As expected, the FeSA+NC@NMPC exhibits an excellent half-wave potential of 0.76 V in 0.1 M phosphate buffer solutions, outperforming that of commercial Pt/C (0.73 V). Theoretical calculations reveal the synergistic effect between atomic Fe-N4 sites and Fe nanoclusters, in which the former possess stable O2 adsorption and rapid intermediate conversion, while the latter facilitates fast water dissociation to supply protons for accelerating the proton-coupled electron transfer process. Moreover, the FeSA+NC@NMPC-based neutral zinc-air batteries afford a high open-circuit potential of 1.42 V and outstanding cycling stability at 5 mA cm−2 for 100 h. This work utilizes the advantages of both single sites and clusters of Fe to provide an in-depth understanding of the neutral ORR mechanism and advances the development of related energy storage and conversion technologies. © 2023 Elsevier B.V.
KW - Fe single atomic sites
KW - Neutral Zinc-air batteries
KW - Oxygen reduction reaction
KW - Synergistic effect
KW - Water dissociation
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UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85171585109&origin=recordpage
U2 - 10.1016/j.cej.2023.146065
DO - 10.1016/j.cej.2023.146065
M3 - RGC 21 - Publication in refereed journal
SN - 1385-8947
VL - 475
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 146065
ER -
