4.8 Article

Highly Conductive Two-Dimensional Metal-Organic Frameworks for Resilient Lithium Storage with Superb Rate Capability

Journal

ACS NANO
Volume 14, Issue 9, Pages 12016-12026

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c05200

Keywords

conductive 2D metal-organic frameworks (MOFs); benzenchexathiolatc; Cu-BHT; LIBs; cathode; high-rate

Funding

  1. Australian Research Council (ARC) Discovery Project [DP160102627, DP1701048343]
  2. AcRF, Singapore [RG 111/17, RG 2/17, RG 114/16, RG 113/18, MOE 2017-T2-1-021, MOE 2018-T2-1-070]
  3. National Key R&D Program of China [2017YFA0204701]
  4. National Natural Science Foundation of China [21790051]

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Redox-active organic cathode materials have drawn growing attention because of the broad availability of raw materials, eco-friendliness, scalable production, and diverse structural flexibility. However, organic materials commonly suffer from fragile stability in organic solvents, poor electrochemical stability in charge/discharge processes, and insufficient electrical conductivity. To address these issues, using Cu(II) salt and benzenehexathiolate (BHT) as the precursors, we synthesized a robust and redox-active 2D metal-organic framework (MOF), [Cu-3(C6S6)](n), namely, Cu-BHT. The Cu-BHT MOFs have a highly conjugated structure, affording a high electronic conductivity of 231 S cm(-1), which could further be increased upon lithiation in lithium-ion battery (LIB) applications. A reversible four-electron reaction reveals the Li storage mechanism of the Cu-BHT for a theoretical capacity of 236 mAh g(-1). The as-prepared Cu- BHT cathode delivers an excellent reversible capacity of 175 mAh g(-1) with ultralow capacity deterioration (0.04890 per cycle) upon 500 cycles at a high current density of 300 mA g(-1). Therefore, we believe this work would provide a practical strategy for the development of high-power energy storage materials.

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