Conductive Holey MoO2–Mo3N2 Heterojunctions as Job-Synergistic Cathode Host with Low Surface Area for High-Loading Li–S Batteries
- Rongrong LiRongrong LiSolid-State Functional Materials Research Laboratory, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, ChinaCenter of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, ChinaMore by Rongrong Li,
- Xuejun ZhouXuejun ZhouState Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, ChinaMore by Xuejun Zhou,
- Hangjia ShenHangjia ShenSolid-State Functional Materials Research Laboratory, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, ChinaMore by Hangjia Shen,
- Minghui Yang*Minghui Yang*E-mail: [email protected]Solid-State Functional Materials Research Laboratory, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, ChinaCenter of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, ChinaMore by Minghui Yang, and
- Chilin Li*Chilin Li*E-mail: [email protected]State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, ChinaCenter of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, ChinaMore by Chilin Li
Abstract
Li–S batteries have several advantages in terms of ultrahigh energy density and resource abundance. However, the insulating nature of S and Li2S, solubility and shuttle effects of lithium polysulfides (LiPSs), and slow interconversion between LiPSs and S/Li2S/Li2S2 are significant impediments to the commercialization of Li–S batteries. Exploration of the advanced S host skeleton simultaneously with high conductivity, adsorbability, and catalytic activity is highly desired. Herein, a heterojunction material with holey nanobelt morphology and low surface area (95 m2/g) is proposed as a compact cathode host to enable a conformal deposition of S/Li2S with homogeneous spatial distribution. The rich heterointerfaces between MoO2 and Mo3N2 nanodomains serve as job-synergistic trapping-conversion sites for polysulfides by combining the merits of conductive Mo3N2 and adsorptive MoO2. This non-carbon heterojunction substrate enables a high S loading of 75 wt % even under low surface area. The initial capacity of MoO2–Mo3N2@S reaches 1003 mAh/g with a small decay rate of 0.024% per cycle during 1000 cycles at 0.5 C. The long-term cyclability is preserved even under a high loading of 3.2 mg/cm2 with a reversible capacity of 451 mAh/g after 1000 cycles. The Li-ion diffusion coefficient for MoO2–Mo3N2@S is extremely high (up to 2.7 × 10–7 cm2/s) benefiting from LiPS conversion acceleration at heterojunctions. The affinity between LiPSs and heterojunction allows a dendrite-free Li plating at anode even after long-term cycling. Well-defined heterointerface design with job-sharing or job-synergic function appears to be a promising solution to high-performance Li–S batteries without the requirement of loose or high-surface-area carbon network structures.
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