Journal
ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 1, Pages 350-356Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.0c02281
Keywords
Battery; Li-ion; naphthalene diimide; covalent organic framework; polymers
Funding
- United States Army Research Office for a Multidisciplinary University Research Initiative (MURI) award [W911NF-15-1-0447]
- MUREP, NASA grant [NNX15A-P44A]
- United States-India Educational Foundation (USIEF, India) [2266/FNPDR/2017]
- Institute of International Education (IIE, USA) [2266/FNPDR/2017]
- Basque Government [MV_2018_1_0012]
- National Science Foundation Graduate Research Fellowship [DGE-1324585]
- National Science Foundation [ECCS-1542174, 0960140]
- Northwestern University
- Dow Chemical Company
- DuPont de Nemours, Inc.
- DOE Office of Science [DE-AC02-06CH11357]
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A two-dimensional imine-linked COF, TAPB-NDI COF, containing NDI redox groups exhibited high theoretical capacity and Faradaic efficiency in lithium-ion batteries. Its large pores facilitated efficient Li+ ion transport, showcasing potential for use in neutral aqueous batteries.
We report a two-dimensional (2D) imine-linked covalent organic framework (COF) containing naphthalene diimide (NDI) redox groups, TAPB-NDI COF. Lithium-ion batteries (LIBs) with TAPB-NDI COF-based electrodes exhibited >95% of their theoretical capacity at a C/20 charge/discharge rate, among the highest faradaic efficiency of a NDI-COF electrode. The pores of TAPB-NDI COF are among the largest reported and presumably facilitate efficient Li+ ion transport. An amorphous cross-linked network (TAPB-NDI Amp) and a linear polymer (PD-NDI Lp) with similar chemical structures demonstrated lower capacities than the COF at C/20 current rate. However, PD-NDI Lp exhibited an overall higher gravimetric capacity and superior specific capacity retention at higher discharge rates compared to the TAPB-NDI COF. The COF is stable in neutral aqueous solutions, allowing its use as an electrode in neutral aqueous LIBs, which exhibited better rate performances than those in coin-cell set ups. Importantly, the cathodes did not suffer from a competitive hydrogen evolution reaction in aqueous LIBs. This opens up opportunities for using NDI moieties in neutral aqueous batteries and other energy-storage devices. Aqueous devices have been largely limited to quinone-hydroquinone-based redox couples, which are, however, operable only in acidic media.
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