纳米团簇
催化作用
X射线吸收光谱法
材料科学
纳米技术
化学工程
氧气
化学
结晶学
吸收光谱法
有机化学
量子力学
物理
工程类
作者
Weijuan Zhai,Senhe Huang,Chenbao Lu,Xiannong Tang,Longbin Li,Bingyu Huang,Ting Hu,Kai Yuan,Xiaodong Zhuang,Yiwang Chen
出处
期刊:Small
[Wiley]
日期:2022-02-26
卷期号:18 (15)
被引量:93
标识
DOI:10.1002/smll.202107225
摘要
Abstract Atomically nitrogen‐coordinated iron atoms on carbon (FeNC) catalysts are emerging as attractive materials to substitute precious‐metal‐based catalysts for the oxygen reduction reaction (ORR). However, FeNC usually suffers from unsatisfactory performance due to the symmetrical charge distribution around the iron site. Elaborately regulating the microenvironment of the central Fe atom can substantially improve the catalytic activity of FeNC, which remains challenging. Herein, N/S co‐doped porous carbons are rationally prepared and are verified with rich Fe‐active sites, including atomically dispersed FeN 4 and Fe nanoclusters (FeSA‐FeNC@NSC), according to systematically synchrotron X‐ray absorption spectroscopy analysis. Theoretical calculation verifies that the contiguous S atoms and Fe nanoclusters can break the symmetric electronic structure of FeN 4 and synergistically optimize 3 d orbitals of Fe centers, thus accelerating OO bond cleavage in OOH* for improving ORR activity. The FeSA‐Fe NC @NSC delivers an impressive ORR activity with half‐wave‐potential of 0.90 V, which exceeds that of state‐of‐the‐art Pt/C (0.87 V). Furthermore, FeSA‐Fe NC @NSC‐based Zn‐air batteries deliver excellent power densities of 259.88 and 55.86 mW cm –2 in liquid and all‐solid‐state flexible configurations, respectively. This work presents an effective strategy to modulate the microenvironment of single atomic centers and boost the catalytic activity of single‐atom catalysts by tandem effect.
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