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Nanostructured Conductive Metal–Organic Frameworks for Sustainable Low Charge Overpotentials in Li–Air Batteries
Summary:
The authors from University of Illinois at Chicago & Argonne National Laboratory developed conductive Cu-THQ MOF nanoflakes that enable Li–O₂ batteries to cycle 100–300 times at 1–2 A g⁻¹ with charge potentials <3.7 V.
Background:
1. To cut high charge overpotentials in Li–O₂ batteries, prior work used carbon or oxide hosts, but insulating Li₂O₂ passivation and poor kinetics remain.
2. The team now proposes a redox-coupled conductive MOF cathode that templates nanocrystalline/amorphous Li₂O₂ and sustains low polarisation.
Research Content:
1. Synthesis: Liquid-phase exfoliation of bulk Cu-THQ into ≈145 nm nanoflakes; coated on GDE without carbon additive.
2. Characterizations:
1) BET: microporous, <1 nm honeycomb pores;
2) TEM: 2–5 nm Li₂O₂ nanocrystals embedded in amorphous Li₂O₂;
3) XPS, EELS, DEMS confirm reversible Li₂O₂ formation/decomposition (e⁻/O₂ ≈ 2).
3. Application: In dry-air Li–O₂ coin cells (1 M LiNO₃ + 0.1 M InBr₃ in TEGDME) the cathode delivers 1000–2000 mAh g⁻¹ at 1–2 A g⁻¹ with ≤1.3 V gap for 100–300 cycles.
4. Mechanism: DFT shows Cu sites nucleate Li₂O₂; conductive MOF + Br⁻ redox mediator allow direct electron transfer across amorphous Li₂O₂, bypassing insulating grain boundaries.
Outlook:
The study proves that intrinsically conductive MOFs can simultaneously template favourable Li₂O₂ morphology and integrate redox mediation, opening a scalable route for high-rate, long-life Li–air batteries.
Nanostructured Conductive Metal–Organic Frameworks for Sustainable Low Charge Overpotentials in Li–Air Batteries
Authors: Leily Majidi, Alireza Ahmadiparidari, Nannan Shan, Sachin Kumar Singh, Chengji Zhang, Zhehao Huang, Sina Rastegar, Khagesh Kumar, Zahra Hemmat, Anh T. Ngo, Peter Zapol, Jordi Cabana, Arunkumar Subramanian, Larry A. Curtiss, Amin Salehi-Khojin
DOI: 10.1002/smll.202102902
Link: https://onlinelibrary.wiley.com/doi/10.1002/smll.202102902
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