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High-Capacity Mg–Organic Batteries Based on Nanostructured Rhodizonate Salts Activated by Mg–Li Dual-Salt Electrolyte

  • Jing Tian
    Jing Tian
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100039, China
    More by Jing Tian
    • , 
  • Dunping Cao
    Dunping Cao
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Dunping Cao
    • , 
  • Xuejun Zhou
    Xuejun Zhou
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Xuejun Zhou
    • , 
  • Jiulin Hu
    Jiulin Hu
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100039, China
    More by Jiulin Hu
    • , 
  • Minsong Huang
    Minsong Huang
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    University of Chinese Academy of Sciences, Beijing 100039, China
    More by Minsong Huang
    • , and 
  • Chilin Li*
    Chilin Li
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    *E-mail: [email protected]
    More by Chilin Li
    Orcidhttp://orcid.org/0000-0002-5587-8617
Cite this: ACS Nano 2018, 12, 4, 3424–3435
Publication Date (Web):April 4, 2018
https://doi.org/10.1021/acsnano.7b09177
Copyright © 2018 American Chemical Society
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Abstract

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A magnesium battery is a promising candidate for large-scale transportation and stationary energy storage due to the security, low cost, abundance, and high volumetric energy density of a Mg anode. But there are still some obstacles retarding the wide application of Mg batteries, including poor kinetics of Mg-ion transport in lattices and low theoretical capacity in inorganic frameworks. A Mg–Li dual-salt electrolyte enables kinetic activation by dominant intercalation of Li-ions instead of Mg-ions in cathode lattices without the compromise of a stable Mg anode process. Here we propose a Mg–organic battery based on a renewable rhodizonate salt (e.g., Na2C6O6) activated by a Mg–Li dual-salt electrolyte. The nanostructured organic system can achieve a high reversible capacity of 350–400 mAh/g due to the existence of high-density carbonyl groups (C═O) as redox sites. Nanocrystalline Na2C6O6 wired by reduced graphene oxide enables a high-rate performance of 200 and 175 mAh/g at 2.5 (5 C) and 5 A/g (10 C), respectively, which also benefits from a high intrinsic diffusion coefficient (10–12–10–11 cm2/s) and pesudocapacitance contribution (>60%) of Na2C6O6 for Li–Mg co-intercalation. The suppressed exfoliation of C6O6 layers by a firmer non-Li pinning via Na–O–C or Mg–O–C and a dendrite-resistive Mg anode lead to a long-term cycling for at least 600 cycles. Such an extraordinary capacity/rate performance endows the Mg–Na2C6O6 system with high energy and power densities up to 525 Wh/kg and 4490 W/kg (based on active cathode material), respectively, exceeding the level of high-voltage insertion cathodes with typical inorganic structures.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.7b09177.

  • SEM images of rhodizonate salts, charge–discharge curves of rhodizonate salts at 0.1–2.0 V, CV of APC–LiCl electrolyte, rate performance of rhodizonate salts, charge–discharge performance of n-SR in an MACC-LiTFSI system, charge–discharge curves of rhodizonate salts in APC and MHCC systems, CV curves of rhodizonate salts, charge–discharge curves of rhodizonate salts for Li batteries, XRD patterns of pristine and cycled n-SR, linear fitting of GITT curve, capacitive effect analysis for b-SR and LR, impedance spectra of Mg/n-SR cells, rate performance comparison of n-SR with different binders, illustration of estimation of energy density value (PDF)

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This article is cited by 36 publications.

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