Mesoporous Yolk-Shell Structured Organosulfur Nanotubes with Abundant Internal Joints for High-Performance Lithium-Sulfur Batteries by Kinetics Acceleration

Although organosulfur compounds can protect lithium anodes, participate in the redox reaction, and suppress the shuttle effect, the sluggish electrochemical dynamics of their bulk structure and the notorious shuttle effect of covalent long-chain sulfurs largely impede their actual applications. Herein, sulfurized carbon nanotube@aminophenol-formaldehyde (SC@A) with covalently linked short-chain sulfurs is firstly synthesized by in situ polymerization of aminophenol-formaldehyde (AF) on the surface of carbon nanotubes (CNTs) followed by acetone etching and inverse sulfurization processes, forming mesoporous yolk-shell organosulfur nanotubes with abundant internal joints between the yolk of CNTs and the shell of sulfurized AF for the first time. In situ Raman spectra, in situ XRD patterns, and ex situ XPS spectra verify that the covalent short-chain sulfurs bring about a reversible solid-solid conversion process of sulfur, thoroughly avoiding the shuttle effect. The mesoporous yolk-shell structure with abundant internal joints can effectively accommodate the volume change, fully expose active sites and efficiently improve the transport of electrons and lithium ions, thus highly promoting the solid-solid electrochemical reaction kinetics. Therefore, the SC@A cathode exhibits a superior specific capacity of 841 mAh g^-1 and a capacity decay of 0.06% per cycle within 500 cycles at a large current density of 5.0 C.