期刊
ACS NANO
卷 14, 期 11, 页码 16022-16035出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c07658
关键词
N-doped Co nanoclusters; hierarchical porous N-doped carbon; catalytic effects; enhanced reaction kinetics; K-S battery
类别
资金
- State Key Program of National Natural Science of China [51532005]
- National Nature Science Foundation of China [51472148, 51272137]
- Tai Shan Scholar Foundation of Shandong Province
- National Youth Science Foundation of China [51702177]
Despite high theoretical capacity and earth-abundant resources, the potential industrialization of potassium-sulfur (K-S) batteries is severely plagued by poor electrochemical reaction kinetics and a parasitic shuttle effect. Herein, a facile low-temperature pyrolysis strategy is developed to synthesize N-doped Co nanocluster inlaid porous N-doped carbon derived from ZIF-67 as catalytic cathodes for K-S batteries. To maximize the utilization efficiency, the size of Co nanoparticles can be tuned from 7 nm to homogeneously distributed 3 nm clusters to create more active sites to regulate affinity for S/polysulfides, improving the conversion reaction kinetics between captured polysulfides and K2S3/S, fundamentally suppressing the shuttle effect. Cyclic voltammetry curves, Tafel plots, electrochemical impedance spectroscopy, and density functional theory calculations ascertain that 3 nm Co clusters in S-N-Co-s-C cathodes exhibit superior catalytic activity to ensure low charge transfer resistance and energy barriers, enhanced exchange current density, and improved conversion reaction rate. The constructed S-N-Co-s-C cathode delivers a superior reversible capacity of 453 mAh g(-1) at 50 mA g(-1) after 50 cycles, a dramatic rate capacity of 415 mAh g(-1) at 400 mA g(-1), and a long cycling stability. This work provides an avenue to make full use of high catalytic Co nanoclusters derived from metal-organic frameworks.
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