Abstract
The development of rechargeable magnesium (Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode. However, the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan, mainly caused by non-uniform distribution of electrodeposits. In this work, a fresh design concept of three-dimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity. A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths. As revealed by finite element simulation and DFT calculation results, the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds. The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed. As a result, an exceptional cycle life of 500 cycles at 4.0 mA cm−2 and 4.0 mA h cm−2 is firstly realized to our best knowledge. Besides, the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm−2 under a normalized capacity of 5.0 mA h cm−2, far exceeding previous results. This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.
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