期刊
ENERGY STORAGE MATERIALS
卷 46, 期 -, 页码 269-277出版社
ELSEVIER
DOI: 10.1016/j.ensm.2021.12.040
关键词
Single-atom catalyst; Coordination environment; Electronic structure; Lithium sulfur battery
资金
- Natural Science Foundation of Hebei Province of China [B2021202028, B2020202052]
- Outstanding Youth Project of Guangdong Natural Science Foundation [2021B1515020051]
- Xijiang RD Team
- Guangdong Innovative and Entrepreneurial Team Program [2016ZT06C517]
- Department of Science and Technology of Guangdong Province [2020B0909030004, 2019JC01L203]
- Science and Technology Program of Guangzhou [2019050001]
- Science and Technology Program of Zhaoqing [2019K038]
- Natural Sciences and Engineering Research Council of Canada
In this study, the deficiency coordination of single-atom Fe site was predicted and validated to enhance sulfur immobilization and catalytic activity, leading to the preparation of a high-performance catalyst for Li-S batteries. The monodispersed FeN2-NC showed excellent electrochemical performance through tuning the coordination number.
The rationally-designed single-atom catalyst that promotes efficient sulfur electrochemistry is highly desired yet still challenging for the development of high-performance lithium-sulfur (Li-S) batteries. Herein, the deficient coordination of single-atom Fe site is firstly and theoretically predicted to endorse higher sulfur affinity and catalytic activity, due to the stronger hybridization between Fe 3d(zz) and S 3p(y) orbitals compared with that in common FeN4 scenario. The following validation is conducted to prepare the monodispersed Fe single atoms with tuned coordination number on nitrogen-doped carbon (denoted as FeN2-NC and FeN4-NC) via the ligand control on the Fe precursor. As expected, the undercoordinated FeN2-NC fulfills significantly stronger sulfur immobilization and catalyzation as confirmed by a series of physicochemical and electrochemical evaluations. As a result, sulfur electrodes hosted by FeN2-NC realize excellent cyclability and rate capability, and particularly, a highly reversible areal capacity up to 4.5 mAh cm(-2) under a high areal sulfur loading of 5.0 mg cm(-2) and a low electrolyte to sulfur ratio of 5.3 mL g(-1). This work highlights the great feasibility and validity of coordinative defect engineering in single-atom catalysts for improving the Li-S battery electrochemistry, which could also enlighten advanced material designs in other related energy areas.
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