TY - JOUR
T1 - Metal/Graphene Composites with Strong Metal-S Bondings for Sulfur Immobilization in Li-S Batteries
AU - Yao, Xiaolong
AU - Xu, Jijian
AU - Hong, Zhanglian
AU - Li, Gaoran
AU - Wang, Xuewei
AU - Lu, Feng
AU - Wang, Weihua
AU - Liu, Hui
AU - Liang, Chengdu
AU - Lin, Zhan
AU - Wang, Weichao
N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].
PY - 2018/2/15
Y1 - 2018/2/15
N2 - Selections of metallic cathode materials and modulations of metal-sulfur bonding strength are crucial for sulfur immobilization in development of high-performance lithium-sulfur (Li-S) batteries with low cost. By combining theoretical calculations and experiments, herein we reveal the relationship between intrinsic electronic structure and metal-S bonding strength, which links to energy density and durability of Li-S batteries. Through first-principles calculations, we simulate sulfur clusters (S1, S2, S4, and S8) immobilization on metal (Cu, Ni, and Sn) slab surfaces with and without graphene substrate. For sulfur clusters, the metal-Sx (x = 1, 2, 4, and 8) bonding strength is in the sequence of Ni > Cu > Sn without graphene substrate. Nevertheless, the sequence changes (Ni > Sn > Cu) in the presence of graphene substrate due to different amounts of charge transfer between these metal clusters and graphene. Guided by these theoretical results, metal (Cu, Ni, Sn)/graphene (G) composites are synthesized and subsequently integrated into the cathode of Li-S batteries. Among these metal/G systems, the sulfur cathode with Ni/G composites demonstrates remarkable electrochemical performance, i.e., a discharge capacity of >830 mAh g-1 over 500 cycles with an average Coulombic efficiency close to 100%. These findings shed light on theoretical calculations providing insights into the electrode design of Li-S batteries. © 2018 American Chemical Society.
AB - Selections of metallic cathode materials and modulations of metal-sulfur bonding strength are crucial for sulfur immobilization in development of high-performance lithium-sulfur (Li-S) batteries with low cost. By combining theoretical calculations and experiments, herein we reveal the relationship between intrinsic electronic structure and metal-S bonding strength, which links to energy density and durability of Li-S batteries. Through first-principles calculations, we simulate sulfur clusters (S1, S2, S4, and S8) immobilization on metal (Cu, Ni, and Sn) slab surfaces with and without graphene substrate. For sulfur clusters, the metal-Sx (x = 1, 2, 4, and 8) bonding strength is in the sequence of Ni > Cu > Sn without graphene substrate. Nevertheless, the sequence changes (Ni > Sn > Cu) in the presence of graphene substrate due to different amounts of charge transfer between these metal clusters and graphene. Guided by these theoretical results, metal (Cu, Ni, Sn)/graphene (G) composites are synthesized and subsequently integrated into the cathode of Li-S batteries. Among these metal/G systems, the sulfur cathode with Ni/G composites demonstrates remarkable electrochemical performance, i.e., a discharge capacity of >830 mAh g-1 over 500 cycles with an average Coulombic efficiency close to 100%. These findings shed light on theoretical calculations providing insights into the electrode design of Li-S batteries. © 2018 American Chemical Society.
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U2 - 10.1021/acs.jpcc.7b12063
DO - 10.1021/acs.jpcc.7b12063
M3 - RGC 21 - Publication in refereed journal
SN - 1932-7447
VL - 122
SP - 3263
EP - 3272
JO - The Journal of Physical Chemistry C
JF - The Journal of Physical Chemistry C
IS - 6
ER -
SDG 7 Affordable and Clean Energy