To cope with the shuttling of soluble lithium polysulfides in lithium–sulfur batteries, confinement tactics, such as trapping of sulfur within porous carbon structures, have been extensively studied. Although performance has improved a bit, the slow polysulfide conversion inducing fast capacity decay remains a big challenge. Herein, a NiS2/carbon (NiS2/C) composite with NiS2 nanoparticles embedded in a thin layer of carbon over the surface of micro-sized hollow structures has been prepared from Ni-metal–organic frameworks. These unique structures can physically entrap sulfur species and also influence their redox conversion kinetics. By improving the reaction kinetics of polysulfides, the NiS2/carbon@sulfur (NiS2/C@S) composite cathode with a suppressed shuttle effect shows a high columbic efficiency and decent rate performance. An initial capacity of 900 mAh g−1 at the rate of 1 C (1 C = 1675 mA g−1) and a low-capacity decline rate of 0.132% per cycle after 500 cycles are obtained, suggesting that this work provides a rational design of a sulfur cathode.
REFERENCES
1.
J.-H.
Shim
, J.-M.
Han
, J.-H.
Lee
, and S.
Lee
, “Mixed electronic and ionic conductor-coated cathode material for high-voltage lithium ion battery
,” ACS Appl. Mater. Interfaces
8
(19
), 12205
–12210
(2016
).2.
H.-J.
Peng
, J.-Q.
Huang
, X.-Y.
Liu
, X.-B.
Cheng
, W.-T.
Xu
, C.-Z.
Zhao
, F.
Wei
, and Q.
Zhang
, “Healing high-loading sulfur electrodes with unprecedented long cycling life: Spatial heterogeneity control
,” J. Am. Chem. Soc.
139
(25
), 8458
–8466
(2017
).3.
H.-J.
Noh
, S.-T.
Myung
, H.-G.
Jung
, H.
Yashiro
, K.
Amine
, and Y.-K.
Sun
, “Formation of a continuous solid‐solution particle and its application to rechargeable lithium batteries
,” Adv. Funct. Mater.
23
(8
), 1028
–1036
(2013
).4.
A.
Manthiram
, Y.
Fu
, S.-H.
Chung
, C.
Zu
, and Y.-S.
Su
, “Rechargeable lithium–sulfur batteries
,” Chem. Rev.
114
(23
), 11751
–11787
(2014
).5.
Y. V.
Mikhaylik
and J. R.
Akridge
, “Polysulfide shuttle study in the Li/S battery system
,” J. Electrochem. Soc.
151
(11
), A1969
–A1976
(2004
).6.
J.
Jiang
, J.
Zhu
, W.
Ai
, X.
Wang
, Y.
Wang
, C.
Zou
, W.
Huang
, and T.
Yu
, “Encapsulation of sulfur with thin-layered nickel-based hydroxides for long-cyclic lithium–sulfur cells
,” Nat. Commun.
6
, 8622
(2015
).7.
Y.-X.
Yin
, S.
Xin
, Y.-G.
Guo
, and L.-J.
Wan
, “Lithium–sulfur batteries: Electrochemistry, materials, and prospects
,” Angew. Chem., Int. Ed.
52
(50
), 13186
–13200
(2013
).8.
X.
Ji
, S.
Evers
, R.
Black
, and L. F.
Nazar
, “Stabilizing lithium–sulphur cathodes using polysulphide reservoirs
,” Nat. Commun.
2
, 325
(2011
).9.
G.
Zhou
, L.
Li
, D.-W.
Wang
, X.-Y.
Shan
, S.
Pei
, F.
Li
, and H.-M.
Cheng
, “A flexible sulfur‐graphene‐polypropylene separator integrated electrode for advanced Li–S Batteries
,” Adv. Mater.
27
(4
), 641
–647
(2015
).10.
C.
Zhao
, L.
Liu
, H.
Zhao
, A.
Krall
, Z.
Wen
, J.
Chen
, P.
Hurley
, J.
Jiang
, and Y.
Li
, “Sulfur-infiltrated porous carbon microspheres with controllable multi-modal pore size distribution for high energy lithium–sulfur batteries
,” Nanoscale
6
(2
), 882
–888
(2014
).11.
S.
Moon
, Y. H.
Jung
, W. K.
Jung
, D. S.
Jung
, J. W.
Choi
, and D. K.
Kim
, “Encapsulated monoclinic sulfur for stable cycling of Li–S rechargeable batteries
,” Adv. Mater.
25
(45
), 6547
–6553
(2013
).12.
L.
Wang
, X.
Li
, Y.
Zhang
, W.
Mao
, Y.
Li
, P. K.
Chu
, A.
Kızılaslan
, Z.
Zheng
, and K.
Huo
, “Subnanometer MoP clusters confined in mesoporous carbon (CMK-3) as superior electrocatalytic sulfur hosts for high-performance lithium–sulfur batteries
,” Chem. Eng. J.
446
(1
), 137050
(2022
).13.
Z.
Zhou
, Z.
Chen
, H.
Lv
, Y.
Zhao
, H.
Wei
, G.
Huai
, R.
Xu
, and Y.
Wang
, “High-entropy nanoparticle constructed porous honeycomb as a 3D sulfur host for lithium polysulfide adsorption and catalytic conversion in Li–S batteries
,” J. Mater. Chem. A
11
, 5883
–5894
(2023
).14.
Z.
Yuan
, H.-J.
Peng
, J.-Q.
Huang
, X.-Y.
Liu
, D.-W.
Wang
, X.-B.
Cheng
, and Q.
Zhang
, “Hierarchical free-standing carbon-nanotube paper electrodes with ultrahigh sulfur-loading for lithium–sulfur batteries
,” Adv. Funct. Mater.
24
(39
), 6105
–6112
(2014
).15.
Y.
Fu
, Y.-S.
Su
, and A.
Manthiram
, “Highly reversible lithium/dissolved polysulfide batteries with carbon nanotube electrodes
,” Angew. Chem., Int. Ed.
52
(27
), 6930
–6935
(2013
).16.
F.
Sun
, J.
Wang
, H.
Chen
, W.
Qiao
, L.
Ling
, and D.
Long
, “Bottom-up catalytic approach towards nitrogen-enriched mesoporous carbons/sulfur composites for superior Li–S cathodes
,” Sci. Rep.
3
, 2823
(2013
).17.
Q.
Pang
, D.
Kundu
, M.
Cuisinier
, and L. F.
Nazar
, “Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium–sulphur batteries
,” Nat. Commun.
5
, 4759
(2014
).18.
Q.
Qu
, T.
Gao
, H.
Zheng
, Y.
Wang
, X.
Li
, X.
Li
, J.
Chen
, Y.
Han
, J.
Shao
, and H.
Zheng
, “Strong surface‐bound sulfur in conductive MoO2 matrix for enhancing Li–S battery performance
,” Adv. Mater. Interfaces
2
(7
), 1500048
(2015
).19.
S. S.
Zhang
and D. T.
Tran
, “Pyrite FeS2 as an efficient adsorbent of lithium polysulphide for improved lithium–sulphur batteries
,” J. Mater. Chem. A
4
(12
), 4371
–4374
(2016
).20.
Y.-J.
Li
, J.-M.
Fan
, M.-S.
Zheng
, and Q.-F.
Dong
, “A novel synergistic composite with multi-functional effects for high-performance Li–S batteries
,” Energy Environ. Sci.
9
(6
), 1998
–2004
(2016
).21.
Z.
Li
, C.
Li
, X.
Ge
, J.
Ma
, Z.
Zhang
, Q.
Li
, C.
Wang
, and L.
Yin
, “Reduced graphene oxide wrapped MOFs-derived cobalt-doped porous carbon polyhedrons as sulfur immobilizers as cathodes for high performance lithium sulfur batteries
,” Nano Energy
23
, 15
–26
(2016
).22.
X.
Zhang
, Z.
Ni
, X.
Bai
, H.
Shen
, Z.
Wang
, C.
Wei
, K.
Tian
, B.
Xi
, S.
Xiong
, and J.
Feng
, “Hierarchical porous N-doped carbon encapsulated fluorine-free MXene with tunable coordination chemistry by one-pot etching strategy for lithium–sulfur batteries
,” Adv. Energy Mater.
13
(29
), 2301349
(2023
).23.
C.
Qi
, H.
Li
, J.
Wang
, C.
Zhao
, C.
Fu
, L.
Wang
, and T.
Liu
, “Metal-organic-framework-Derived porous carbon embedded with TiO2 nanoparticles as a cathode for advanced lithium–sulfur batteries
,” ChemElectroChem
8
(1
), 90
–95
(2021
).24.
C.
Qi
, L.
Xu
, J.
Wang
, H.
Li
, C.
Zhao
, L.
Wang
, and T.
Liu
, “Titanium-containing metal–organic framework modified separator for advanced lithium–sulfur batteries
,” ACS Sustainable Chem. Eng.
8
(34
), 12968
–12975
(2020
).25.
D.
Senthil Raja
, C.-C.
Cheng
, Y.-C.
Ting
, and S.-Y.
Lu
, “NiMo-MOF-derived carbon-armored Ni4Mo alloy of an interwoven nanosheet structure as an outstanding pH-universal catalyst for hydrogen evolution reaction at high current densities
,” ACS Appl. Mater. Interfaces
15
(16
), 20130
–20140
(2023
).26.
A. E.
Baumann
, R. I.
Anayah
, and V. S.
Thoi
, “Phosphorus-functionalized organic linkers promote polysulfide retention in MOF-based Li–S batteries
,” ACS Appl. Energy Mater.
5
(12
), 15302
–15309
(2022
).27.
Y.
Guo
, J.
Li
, G.
Yuan
, J.
Guo
, Y.
Zheng
, Y.
Huang
, Q.
Zhang
, J.
Li
, J.
Shen
, C.
Shu
, J.
Xu
, Y.
Tang
, W.
Lei
, and H.
Shao
, “Elucidating the volcanic-type catalytic behavior in lithium–sulfur batteries via defect engineering
,” ACS Nano
17
(18
), 18253
–18265
(2023
).28.
F.
Zou
, Y.-M.
Chen
, K.
Liu
, Z.
Yu
, W.
Liang
, S. M.
Bhaway
, M.
Gao
, and Y.
Zhu
, “Metal organic frameworks derived hierarchical hollow NiO/Ni/graphene composites for lithium and sodium storage
,” ACS Nano
10
(1
), 377
–386
(2016
).29.
R.
Bi
, C.
Zeng
, H.
Huang
, X.
Wang
, and L.
Zhang
, “Metal–organic frameworks derived hollow NiS2 spheres encased in graphene layers for enhanced sodium-ion storage
,” J. Mater. Chem. A
6
(29
), 14077
–14082
(2018
).30.
J.
Li
and H. C.
Zeng
, “Hollowing Sn-doped TiO2 nanospheres via Ostwald ripening
,” J. Am. Chem. Soc.
129
(51
), 15839
–15847
(2007
).© 2024 Author(s). Published under an exclusive license by AIP Publishing.
2024
Author(s)
You do not currently have access to this content.
