High Capacity, Dendrite‐Free Growth, and Minimum Volume Change Na Metal Anode

Na metal anode attracts increasing attention as a promising candidate for Na metal batteries (NMBs) due to the high specific capacity and low potential. However, similar to issues faced with the use of Li metal anode, crucial problems for metallic Na anode remain, including serious moss‐like and dendritic Na growth, unstable solid electrolyte interphase formation, and large infinite volume changes. Here, the rational design of carbon paper (CP) with N‐doped carbon nanotubes (NCNTs) as a 3D host to obtain Na@CP‐NCNTs composites electrodes for NMBs is demonstrated. In this design, 3D carbon paper plays a role as a skeleton for Na metal anode while vertical N‐doped carbon nanotubes can effectively decrease the contact angle between CP and liquid metal Na, which is termed as being “Na‐philic.” In addition, the cross‐conductive network characteristic of CP and NCNTs can decrease the effective local current density, resulting in uniform Na nucleation. Therefore, the as‐prepared Na@CP‐NCNT exhibits stable electrochemical plating/stripping performance in symmetrical cells even when using a high capacity of 3 mAh cm−2 at high current density. Furthermore, the 3D skeleton structure is observed to be intact following electrochemical cycling with minimum volume change and is dendrite‐free in nature. Carbon paper (CP) with N‐doped carbon nanotubes (NCNTs) is rationally designed as a 3D host for Na metal anode. The contact angle between the CP and liquid metal Na is effectively reduced with the vertical N‐doped carbon nanotubes. As‐prepared Na@CP‐NCNTs exhibit stable electrochemical plating/stripping performance in symmetrical cells operated at high current density and high capacity.