Regulating the intrinsic electronic structure of carbon nanofibers with high-spin state Ni for sodium storage with high-power density

Carbon nanofibers (CNFs) with high specific surface area show great potential for sodium storage as a hard carbon material. Herein, CNFs anchored with Ni nanoparticles (CNFs/Ni) were prepared through chemical vapor deposition and impregnation reduction methods, in situ growing on the threedimensional porous copper current collector (3DP-Cu). The coupling effect of high-spin state Ni nanoparticles leads to the increase of defect density and the expansion of lattice spacing of CNFs. Meanwhile, the 3DP-Cu ensures a high loading capacity of CNFs and short ion/electron transport channels. As an integral binder-free anode, the 3DP-Cu/CNFs/Ni exhibits excellent electrochemical performance, which demonstrates a high specific capacity with 298.5 mAh g -1 at 10 0 0 mA g -1 after 1500 cycles, and a high power density with 200 mAh g -1 over 10 0 0 cycles at 50 0 0 mA g -1 . Density functional theory calculation results show that the high-spin state Ni regulates the electronic structure of CNFs, which significantly reduces the adsorption energy for Na+ (-2.7 Ev) and thus enables high-rate capability. The regulation of the electronic structure of carbon materials by high-spin state metal provides a new strategy for developing high-power carbonaceous anode materials for sodium-ion batteries.& COPY; 2023 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.