Journal
ACS NANO
Volume 14, Issue 10, Pages 14057-14069Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c06690
Keywords
potassium-ion batteries; hard carbon anodes; phosphorus/nitrogen cofunctionalized; phosphatylation; porous carbon monoliths; high initial Coulombic efficiency
Categories
Funding
- innovation team project for Climbing Program of Shandong University [2019-05]
- Research Award Fund for Shandong Province Excellent Innovation Team [2012136]
- program for Outstanding Ph.D. candidate of Shandong University
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A hard carbon material with free-standing porous structure and high contents of heteroatom functional groups is considered to be a potential anode for potassium-ion batteries (PIBs). Herein, a free-standing phosphorus/nitrogen cofunctionalized porous carbon monolith (denoted as PN-PCM) anode for PIBs is successfully fabricated via a supercritical CO2 foaming technology, followed by amidoximation, phosphorylation, and thermal treatment. Thanks to the synergistic effect of a three-dimensional macroporous open structure and high P/N contents of 6.19/5.74 at%, the PN-PCM anode delivers an excellent reversible specific capacity (396 mA h g(-1) at 0.1 A g(-1) after 300 cycles) with high initial Coulombic efficiency (63.6%), a great rate performance (168 mA h g(-1) at 5 A g(-1)), and an ultralong cycling stability (218 mA h g(-1) at 1 A g(-1) after 3000 cycles). Theoretical calculations clarify that in a P/N cofunctionalized carbon, the P-C bonds devote more to enhancing the potassium storage via adsorption and improving electronic conductivity of carbon, while P-O bonds contribute more to enlarging the interlayer distance of carbon and reducing the ion diffusion barrier.
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