American Chemical Society
nl9b05349_si_003.mp4 (3.25 MB)

Ultrahigh and Durable Volumetric Lithium/Sodium Storage Enabled by a Highly Dense Graphene-Encapsulated Nitrogen-Doped Carbon@Sn Compact Monolith

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posted on 2020-02-06, 17:03 authored by Yunyong Li, Changzhi Ou, Junlu Zhu, Zhonggang Liu, Jianlin Yu, Wenwu Li, Haiyan Zhang, Qiaobao Zhang, Zaiping Guo
Tin-based composites hold promise as anodes for high-capacity lithium/sodium-ion batteries (LIBs/SIBs); however, it is necessary to use carbon coated nanosized tin to solve the issues related to large volume changes during electrochemical cycling, thus leading to the low volumetric capacity for tin-based composites due to their low packing density. Herein, we design a highly dense graphene-encapsulated nitrogen-doped carbon@Sn (HD N–C@Sn/G) compact monolith with Sn nanoparticles double-encapsulated by N–C and graphene, which exhibits a high density of 2.6 g cm–3 and a high conductivity of 212 S m–1. The as-obtained HD N–C@Sn/G monolith anode exhibits ultrahigh and durable volumetric lithium/sodium storage. Specifically, it delivers a high volumetric capacity of 2692 mAh cm–3 after 100 cycles at 0.1 A g–1 and an ultralong cycling stability exceeding 1500 cycles at 1.0 A g–1 with only 0.019% capacity decay per cycle in lithium-ion batteries. Besides, in situ TEM and ex situ SEM have revealed that the unique double-encapsulated structure effectively mitigates drastic volume variation of the tin nanoparticles during electrode cycling. Furthermore, the full cell using HD N–C@Sn/G as an anode and LiCoO2 as a cathode displays a superior cycling stability. This work provides a new avenue and deep insight into the design of high-volumetric-capacity alloy-based anodes with ultralong cycle life.