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5. A Vacuum Vapor Deposition Strategy to Fe Single‐Atom Catalysts with Densely Active Sites for High‐Performance Zn–Air Battery.

Author

Yang, Xiang, Zhu, Baohui, Gao, Zhiyang, Yang, Can, Zhou, Jingbo, Han, Aijuan, and Liu, Junfeng

Subjects
IRON catalysts, VAPOR-plating, VACUUM deposition, OXYGEN reduction, CHARGE transfer
Abstract

Iron single‐atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N‐doped carbon nanosheets with densely active sites (FeSAs‐UNCNS). Experimental analyses confirm that the FeSAs‐UNCNS achieves densely accessible active sites (1.11 × 1020 sites g−1) in the configuration of Fe─N4O. Consequently, the half‐wave potential of FeSAs‐UNCNS in 0.1 m KOH reaches a remarkable value of 0.951 V versus RHE. Moreover, when employed as the cathode of various kinds of Zn–air batteries, FeSAs‐UNCNS exhibits boosting performances by achieving a maximum power density of 306 mW cm−2 and long cycle life (>180 h) at room temperature, surpassing both Pt/C and reported SACs. Further investigations reveal that FeSAs‐UNCNS facilitates the mass and charge transfer during catalysis and the atomic configuration favors the desorption of *OH kinetically. [ABSTRACT FROM AUTHOR]

Published
2024
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15. Boosting ORR performance by single atomic divacancy Zn–N3C–C8sites on ultrathin N-doped carbon nanosheets

Author

Zhang, Tianyu, Wang, Fanping, Yang, Can, Han, Xu, Liang, Chen, Zhang, Zedong, Li, Yaping, Han, Aijuan, Liu, Junfeng, and Liu, Bin

Abstract

Single-atom catalysts (SACs) show great promise to improve the performance of catalysis because of their spatially isolated single-atom sites with unique electronic properties. Herein, we construct single Zn atoms anchored on ultrathin two-dimensional (2D) N-doped carbon nanosheets (Zn–SAs/UNCNS) as an efficient electrocatalyst for oxygen reduction reaction (ORR). The microenvironment of Zn–SAs/UNCNS with super ORR intrinsic activity was identified as the divacancy Zn–N3C–C8by both experiments and theoretical simulations. Density functional theory (DFT) calculations reveal that the divacancy Zn–N3C–C8sites exhibit near-Fermi electronic states distinct from those of graphene-enclosed Zn–N4–C10and divacancy trans-Zn–N2C2–C8sites, which greatly facilitate the ORR process. Furthermore, compared with 3D architecture, the single atomic divacancy Zn–N3C–C8sites anchored on ultrathin 2D carbon nanosheets show more active site exposure and fast electron transport, which collectively boost the ORR performance, showing a high half-wave potential of 0.91 V versus reversible hydrogen electrode [RHE] and a super turnover frequency (4.99 e−site−1s−1).

Published
2022
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