Edge-nitrogen synergize with micropores to realize fast and durable potassium storage for carbon anode

Abstract

Edge-N (pyridinic/pyrrolic-N) functionalized carbon is a promising anode for potassium-ion batteries, while micropores have been proven to be effective in increasing capacity and cyclability. However, the obtained carbon materials usually exhibit a low N-doping level and edge-N species based on the conventional pyrolysis method, and the exploration of the synergistic effect of edge-N doping and micropores on the potassium-storage performance is still lacking. Herein, a novel strategy is proposed to prepare edge-N doped carbon (ENC-850) by directly pyrolyzing supermolecule precursors self-assembled by terephthalic acid (BDC) and melamine (MA). Because the s-triazine structure in MA is more stable than BDC, which can easily ensure a higher N-doping content in carbon, and the decomposition of s-triazine structure is accompanied by the release of NCNH2 gas, which enables most doped N-atoms to be of edge-N configurations, favoring the adsorption storage of K-ions. Besides, the released small molecules can create numerous micropores, not only providing active sites, but accommodating volume fluctuation. Therefore, the optimized ENC-850 with the most suitable edge-N content of 60.6% (7.73 at% of total 11.71 at% N-doping) and micropores delivers a high capacity (280 mAh g−1 at 0.5 A g−1) and superior cycling stability (over 2000 cycles).