4.8 Article

Metal-Organic Framework Glass Anode with an Exceptional Cycling-Induced Capacity Enhancement for Lithium-Ion Batteries

Journal

ADVANCED MATERIALS
Volume 34, Issue 10, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202110048

Keywords

anode; capacity enhancement; lithium-ion batteries; metal-organic framework crystal; metal-organic framework glass

Funding

  1. China Scholarship Council [201707040085]
  2. Taishan Young Scholarship Project of Shandong Province [tsqn202103098]
  3. Shandong Provincial Natural Science Foundation [ZR2020ME025]
  4. Colleges and Universities Twenty Terms Foundation of Jinan City [2019GXRC034]
  5. State Key Laboratory of Special Glass of China
  6. DOE Office of Science [DE-AC02-06CH11357]

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A MOF glass anode for lithium-ion batteries (LIBs) has been developed, demonstrating high lithium storage capacity, outstanding cycling stability, and superior rate performance. The lithium storage capacity of the MOF glass anode continuously increases with charge-discharge cycling, attributed to the increased distortion and local breakage of the Co-N coordination bonds.
Metal-organic frameworks (MOFs) hold great promise as high-energy anode materials for next-generation lithium-ion batteries (LIBs) due to their tunable chemistry, pore structure and abundant reaction sites. However, the pore structure of crystalline MOFs tends to collapse during lithium-ion insertion and extraction, and hence, their electrochemical performances are rather limited. As a critical breakthrough, a MOF glass anode for LIBs has been developed in the present work. In detail, it is fabricated by melt-quenching Cobalt-ZIF-62 (Co(Im)(1.75)(bIm)(0.25)) to glass, and then by combining glass with carbon black and binder. The derived anode exhibits high lithium storage capacity (306 mAh g(-1) after 1000 cycles at of 2 A g(-1)), outstanding cycling stability, and superior rate performance compared with the crystalline Cobalt-ZIF-62 and the amorphous one prepared by high-energy ball-milling. Importantly, it is found that the Li-ion storage capacity of the MOF glass anode continuously rises with charge-discharge cycling and even tripled after 1000 cycles. Combined spectroscopic and structural analyses, along with density functional theory calculations, reveal the origin of the cycling-induced enhancement of the performances of the MOF glass anode, that is, the increased distortion and local breakage of the Co-N coordination bonds making the Li-ion intercalation sites more accessible.

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