Summary
Here, carbon nanotubes (CNTs) growing on the Ni2P@carbon (Ni2P@C/CNTs) was prepared by Ni‐MOFs as a precursor through pyrolysis combined with phosphorization strategy. As lithium‐ion batteries (LIBs) anode, the as‐prepared Ni2P@C/CNTs presented an outstanding initial discharge capacity (652 mA h g−1) and reversible capacity (442 mA h g−1) after 300 cycles at 0.2 A g−1. The capacity still maintained 252 mA h g−1 at the current density of 1 A g−1. The porous carbon and CNTs growing on carbon spheres enhanced the electrochemical conductivity of the sample, restricted the volume and structural deformation of Ni2P during the discharge/charging process, provided more paths for the movements of Li+ ions/electrons and enlarged the area for electrolyte/Ni2P active materials contacting each other. The results demonstrated that the prominent performances of Ni2P@C/CNTs were ascribed to structural design and paved the way to design other transition metal phosphides‐based anode materials with desired electrochemical performance.