TY - JOUR
T1 - Universal Synthesis of Half-Metallic Diatomic Catalysts for Efficient Oxygen Reduction Electrocatalysis
AU - Yao, Yuechao
AU - Jiang, Tao
AU - Lim, Sung Yul
AU - Frandsen, Cathrine
AU - Li, Zhangjian
AU - Dou, Yibo
AU - Wu, Feiyan
AU - Qin, Jibo
AU - Zou, Jizhao
AU - Stamate, Eugen
AU - Zhang, Wenjing
PY - 2023
Y1 - 2023
N2 - Developing efficient and low-cost noble-free metal electrocatalysts is an urgent requirement. Herein, a one-step, solid-state template-assisted method for fabricating isolated half-metallic diatomic M, Zn─N─C (M═Fe, Co, and Ni) catalysts is reported. In particular, the fabricated Fe, Zn─N─C structure exhibits superior oxygen reduction reaction capabilities with a half-wave potential of 0.867 V versus RHE. The Mossbauer spectra reveal that the Fe, Zn─N─C half-metallic diatomic catalyst has a large proportion of the D2 site (ferrous iron with a medium spin state). Density functional theory (DFT) reveals that in Fe, Zn─N─C structures, the zinc sites play a unique role in accelerating the protonation process of O2 in ORR. In assembled zinc-air batteries, a maximum power density of 138 mW cm-2 and a capacity of 748 mAh g zn-1 can be obtained. This work fabricates a series of efficient M, Zn─N─C diatomic electrocatalysts, and the developed solid-state reaction method can hopefully apply in other energy conversion and storage fields.
AB - Developing efficient and low-cost noble-free metal electrocatalysts is an urgent requirement. Herein, a one-step, solid-state template-assisted method for fabricating isolated half-metallic diatomic M, Zn─N─C (M═Fe, Co, and Ni) catalysts is reported. In particular, the fabricated Fe, Zn─N─C structure exhibits superior oxygen reduction reaction capabilities with a half-wave potential of 0.867 V versus RHE. The Mossbauer spectra reveal that the Fe, Zn─N─C half-metallic diatomic catalyst has a large proportion of the D2 site (ferrous iron with a medium spin state). Density functional theory (DFT) reveals that in Fe, Zn─N─C structures, the zinc sites play a unique role in accelerating the protonation process of O2 in ORR. In assembled zinc-air batteries, a maximum power density of 138 mW cm-2 and a capacity of 748 mAh g zn-1 can be obtained. This work fabricates a series of efficient M, Zn─N─C diatomic electrocatalysts, and the developed solid-state reaction method can hopefully apply in other energy conversion and storage fields.
KW - Dual atoms
KW - Half-metallic diatomic catalysts
KW - Oxygen reduction reaction (ORR)
KW - Zinc-air batteries
U2 - 10.1002/smll.202304655
DO - 10.1002/smll.202304655
M3 - Journal article
C2 - 37590396
SN - 1613-6810
VL - 19
JO - Small
JF - Small
IS - 49
M1 - 2304655
ER -