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ACS Appl Mater Interfaces. 2017 Sep 6;9(35):29829-29838. doi: 10.1021/acsami.7b09363. Epub 2017 Aug 25.

Ultrathin Manganese-Based Metal-Organic Framework Nanosheets: Low-Cost and Energy-Dense Lithium Storage Anodes with the Coexistence of Metal and Ligand Redox Activities.

Author information

1
State Key Laboratory of Precision Spectroscopy, Shanghai Key Laboratory of Magnetic Resonance, Institute of Functional Materials, School of Physics and Materials Science, East China Normal University , Shanghai 200062, P.R. China.
2
Anhui Key Laboratory of Condensed Matter Physics at Extreme Conditions, High Magnetic Field Laboratory, Chinese Academy of Sciences , Hefei 230031, P.R. China.
3
National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei 230029, P.R. China.

Abstract

We herein demonstrate the fabrication of Mn- and Ni-based ultrathin metal-organic framework nanosheets with the same coordination mode (termed "Mn-UMOFNs" and "Ni-UMOFNs", respectively) through an expedient and versatile ultrasonic approach and scrutinize their electrochemical properties as anode materials for rechargeable lithium batteries for the first time. The obtained Mn-UMOFNs with structure advantages over Ni-UMOFNs (thinner nanosheets, smaller metal-ion radius, higher specific surface area) exhibit high reversible capacity (1187 mAh g-1 at 100 mA g-1 for 100 cycles), excellent rate capability (701 mAh g-1 even at 2 A g-1), rapid Li+ diffusion coefficient (2.48 × 10-9 cm2 s-1), and a reasonable charge-discharge profile with low average operating potential at 0.4 V. On the grounds of the low-cost and environmental benignity of Mn metals and terephthalic acid linkers, our Mn-UMOFNs show alluring promise as a low-cost high-energy anode material for future LIBs. Furthermore, the lithiation-delithiation chemistry of Mn-UMOFNs was unequivocally studied by a combination of magnetic measurements, electron paramagnetic resonance, and synchrotron-based soft X-ray spectroscopy (O K-edge and Mn L-edge) experiments, the results of which substantiate that both the aromatic chelating ligands and the Mn2+ centers participate in lithium storage.

KEYWORDS:

local environment; manganese; metal−organic framework; rehybridization; ultrathin nanosheets

PMID:
28812873
DOI:
10.1021/acsami.7b09363

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