Abstract

Inferior specific capacity and sluggish redox kinetics are the most stubborn problems lithium-ion and lithium-sulfur batteries (LIBs and LSBs) are facing, respectively. Here we report a facile fabrication of self-supported hollow Co 3 O 4 @carbon nanotubes on carbon cloth (H-Co 3 O 4 @CNT/CC) through a mild pyrolysis-oxidation process. The additive- and binder-free H-Co 3 O 4 @CNT/CC shows excellent electrochemical performances as both LIBs and LSBs electrodes. As a robust integrated anode for LIBs, the areal capacities are 2.72 mAh cm −2 at the current density of 0.5 C over 1000 cycles. While as a durable cathode host for LSBs, favorable areal capacities of 2.37 mAh cm −2 are maintained with a low capacity decay of 0.11 % per cycle at the sulfur loading of 6 mg cm −2 and current density of 1 C after 400 cycles. Electrochemical technology, ex situ Raman spectroscopy and DFT calculations are performed to comprehensively analyze H-Co 3 O 4 @CNT/CC via thermodynamics and kinetics. It is demonstrated that the hierarchically hollow interior structure, strong adsorb ability of Co 3 O 4 toward polysulfides and three-dimensional (3D) inter-connected conductive carbon framework are responsible for the high areal capacity, fast redox kinetics and cycling durability. The synergistic effect of different components and structures of hollow-Co 3 O 4 @CNT, which have internal hollow structure, incorporation of Co 3 O 4 into elastic buffering framework and high porosity, contributes greatly to the superior electrochemical performances in terms of high areal capacity, good rate capability and ultralong cycling stability. • The integrated electrode possesses the merits of hollow nanostructured Co 3 O 4 and 3D inter-connected conductive network. • Electrochemical technology and DFT calculations are performed to comprehensively analyze H-Co 3 O 4 @CNT/CC. • H-Co 3 O 4 @CNT/CC delivers high areal capacities of 2.72 mAh cm -2 after 1000 cycles at 0.5 C as anode.

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