期刊
ENERGY STORAGE MATERIALS
卷 45, 期 -, 页码 370-379出版社
ELSEVIER
DOI: 10.1016/j.ensm.2021.12.006
关键词
Li-S batteries; Interface; Integrated membrane; MO; Synergistic catalysis
资金
- Natural Science Foundation of China [21676043, 21506028, 21706023]
- National Key Research and Development Program of China [2019YFE0119200]
- Liaoning Natural Science Foundation [2021-MS-116]
- Science Fund for Creative Research Groups of the National Natural Science Foundation of China [22021005]
- Dalian Innovation Funding supporting [2019J12SN68]
- Liaoning Revitalization Talents Program [XLYC2007040]
- Liaoning BaiQianWan Talents Program
- Fundamental Research Funds for the Central Universities [DUT21YG113]
A scalable integrated electrode-separator membrane with hierarchical porous interface is reported for promoting Li+/electrolyte transfer and refining the Li-S battery configuration without aluminum, showing significant potential for improving battery performance.
Herein, scalable integrated electrode-separator membranes with hierarchical porous interface are reported for promoting Li+/electrolyte transfer and Al-free refined Li-S battery configuration. The electrode side (CNT@Mo-NC) with ultrahigh porosity of 89% is composed with CNT as skeleton and Mo/N-codoped carbon (Mo-NC) as the crosslinked shell, the unique porous membrane electrode side and interface can strengthen transfer of Li+/electrons/electrolyte for fast reaction kinetics, and provide large space for polysulfide (LiPSs) anchoring and volume expansion. Furthermore, the N active sites with Li+-transfer transition function and Mo clusters with LiPSs adsorption and catalytic ability constitute a highly-efficient synergistic effect in mitigating shuttle effect and reducing energy barrier of redox reaction. For the Mo-13-NC-a surface with adjacent Mo and N, the LiPSs are adsorbed by Mo during the discharge process, and the N sites with lone electron pairs can accelerate diffusion of the positively charged Li+ to Mo, and to react quickly with LiPSs and transform into Li2S. For Mo-13-NC-b surface, however, the repulsion effect between Mo and Li+ during the charge process can promote the rapid migration of the dissociated Li+ to surround graphene due to the N center is occupied by Mo, which is beneficial to the dissociation reaction of Li2S. For the separator side (CNT@NP) with CNT as the skeleton and nonconductive polymer (NP) as crosslinked shell, the porous structure also facilitates the Li+/electrolyte transport. With uniform sulfur loading in the electrode side, an Al/Cu free Li-S battery with refined configuration and long-term cycle stability is formed. The proposed strategy has an important guiding significance for the design of membrane-based electrode/separator/interlayer with low ion/electrolyte transfer resistance in Li-S batteries.
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