Citation: Shixin SHI, Zhuohang LIU, Yuan SUN, Jingshen LI, Weixiang CHEN. Synthesis and electrochemical lithium storage performance of high-entropy NiCoSnZnFeS_x and reduced graphene oxide composite[J]. Chinese Journal of Inorganic Chemistry, ;2026, 42(9): 1984-1996. doi: 10.11862/CJIC.20250372 shu

Synthesis and electrochemical lithium storage performance of high-entropy NiCoSnZnFeS_x and reduced graphene oxide composite

Shixin SHI ^{1, #} ,
Zhuohang LIU ^{1, #} ,
Yuan SUN ² ,
Jingshen LI ¹ ,
Weixiang CHEN ^1,,

1.
Department of Chemistry, Zhejiang University, Hangzhou 310058, China
2.
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China

Corresponding author: Weixiang CHEN, weixiangchen@zju.edu.cn
Received Date: 13 December 2025
Revised Date: 27 July 2026

Figures(8)

High entropy multicomponent metal sulfide (NiCoSnZnFeS_x) and reduced graphene oxide (rGO) composite (NiCoSnZnFeS_x-rGO) was prepared by a one-step hydrothermal reaction method. Its microstructure, morphology, and electrochemical lithium storage performance were characterized and investigated. It was found that NiCoSnZnFeS_x nanoparticles exhibited the hybrid nanocrystalline structure and were well dispersed on the surface of rGO. As the conversion-type electrode material, NiCoSnZnFeS_x-rGO composite possessed multiple redox pairs for electrochemical lithium storage and could undergo lithiation/delithiation in sequence, which effectively mitigated volume changes of active material during charge/discharge cycles, thereby singnificantly enhancing the cyclic stability. The diversity and interaction of constituent elements in the high-entropy composite improved the electronic conductivity and ionic diffusion, which could enhance high-rate capability. Therefore, the NiCoSnZnFeS_x-rGO composite exhibited the excellent electrochemical lithium storage performance. It could deliver an initial reversible specific capacity as high as 1 230 mAh·g^-1 at the current density of 0.1 A·g^-1 and exhibited good high-rate capability of 869 mAh·g^-1 at 2.0 A·g^-1. After 900 cycles, it still maintained a reversible specific capacity of 996 mAh·g^-1 at 1.0 A·g^-1, demonstrating its stable long-cycle performance. The excellent electrochemical lithium storage performance of NiCoSnZnFeS_x-rGO is mainly due to that the diversity of its constituent elements and the synergistic effect of different metal sulfides significantly enhance the conversion reaction reversibility of electrochemical lithium storage and the cyclic stability.
- electrochemical lithium storage,
- NiCoSnZnFeS_x,
- reduced graphene oxides,
- high entropy,
- hydrothermal reaction
1. [1]
  SEO J W, JANG J T, PARK S W, KIM C, PARK B, CHEON J. Two-dimensional SnS₂ nanoplates with extraordinary high discharge capacity for lithium ion batteries[J]. Adv. Mater., 2008, 20: 4269-4273 doi: 10.1002/adma.200703122
2. [2]
  XU C, JING Y, HE J R, ZHOU K R, CHEN Y F, LI Q, LIN J, ZHANG W L. Self-assembled interwoven CoS₂/CNTs/graphene architecture as anode for high-performance lithium ion batteries[J]. J. Alloy. Compd., 2017, 708: 1178-1183 doi: 10.1016/j.jallcom.2017.03.099
3. [3]
  YANG D D, ZHAO M, ZHANG R D, ZHANG Y, YANG C C, JIANG Q. NiS₂ nanoparticles anchored on open carbon nanohelmets as an advanced anode for lithium-ion batteries[J]. Nanoscale Adv., 2020, 2: 512-519 doi: 10.1039/C9NA00661C
4. [4]
  XU G, JIANG X N, CHEN W X. Preparation of ZnS@C/rGO composite for electrochemical reversible lithium storage[J]. Chinese J. Inorg. Chem., 2022, 38: 891-900
5. [5]
  BI R, ZENG C, HUANG H, WANG X, ZHANG L. Metal-organic frameworks derived hollow NiS₂ spheres encased in graphene layers for enhanced sodium-ion storage[J]. J. Mater. Chem. A, 2018, 6: 14077-14082 doi: 10.1039/C8TA05554H
6. [6]
  CHANG K, WANG Z, HUANG G C, LI H, CHEN W X, LEE J Y. Few-layer SnS₂/graphene hybrid with exceptional electrochemical performance as lithium-ion battery anode[J]. J. Power Sources, 2012, 201: 259-266 doi: 10.1016/j.jpowsour.2011.10.132
7. [7]
  LI H, HE Y Y, DAI Y X, REN Y Q, GAO T T, ZHOU G W. Bimetallic SnS₂/NiS₂@S-rGO nanocomposite with hierarchical flower-like architecture for superior high rate and ultra-stable half/full sodium-ion batteries[J]. Chem. Eng. J., 2022, 427: 131784 doi: 10.1016/j.cej.2021.131784
8. [8]
  CHANG K, Chen W X. L-cysteine-assisted synthesis of layered MoS₂/graphene composites with excellent electrochemical performances for lithium ion batteries[J]. ACS Nano, 2011, 5(6): 4720-4728 doi: 10.1021/nn200659w
9. [9]
  CHEN Q N, CHEN W X, YE J B, WANG Z, LEE J Y. L-cysteine- assisted hydrothermal synthesis of nickel disulfide/graphene composite with enhanced electrochemical performance for reversible lithium storage[J], J. Power Sources, 2015, 294: 51-58 doi: 10.1016/j.jpowsour.2015.06.071
10. [10]
  LIU X Q, XIANG Y, LI Q P, ZHENG Q J, JIANG N, HUO Y, LIN D M. SnS₂-CoS₂@C nanocubes as high initial Coulombic efficiency and long-life anodes for sodium-ion batteries[J]. Electrochim. Acta, 2021, 387: 138525 doi: 10.1016/j.electacta.2021.138525
11. [11]
  PAN P, CHEN L H, DING Y, DU J, FENG C Q, FU Z B, QIN C Q, WANG F. Nitrogen-doped carbon decorated Cu₂NiSnS₄ microflowers as superior anode materials for long-life lithium-ion batteries[J]. J. Solid State Chem., 2018, 261: 103-110 doi: 10.1016/j.jssc.2018.02.021
12. [12]
  PENG K, ZHAO X Y, CHEN Z Q, ZHANG X H, ZENG Y Q, JIANG J Q. Progress in the application of high-entropy alloys and high- entropy ceramics in water electrolysis[J]. Chinese J. Inorg. Chem., 2025, 41: 1257-1275
13. [13]
  CHE C J, BI J Q, ZHANG X H, YANG Y, WANG H Y, RONG J C. Synthesis and electrochemical performance of novel high-entropy spinel oxide (FeCoMgCrLi)₃O₄[J]. J. Electroanal. Chem., 2024, 974: 137521
14. [14]
  CHENG W B, LIU J, HU J, PENG W F, NIU G L, LI J K, CHENG Y, FENG X L, FANG L M, WANG M S, REDFERN S, TANG M X, WANG G K, GOU H Y. Pressure‑stabilized high‑entropy (FeCoNiCuRu)S₂ sulfide anode toward simultaneously fast and durable lithium/sodium ion storage[J]. Small, 2023, 19: 202301915
15. [15]
  LIN L, WANG K, SARKAR A, NJEL C, KARKERA G, WANG Q S, AZMI R, FICHTNER M, HAHN H, SCHWEIDLER S, BREITUNG B. High-entropy sulfides as electrode materials for Li-ion batteries[J]. Adv. Energy Mater., 2022, 12: 2103090 doi: 10.1002/aenm.202103090
16. [16]
  SHU J Y, SI Y C, MA X L, LEI W L, ZHAO Y M, SHAN C S. High entropy metal sulfide stabilized by ZIF-8-derived carbon as high- performance anode in lithium ion battery[J]. Carbon, 2025, 238: 120166 doi: 10.1016/j.carbon.2025.120166
17. [17]
  XU H Y, WANG R, KANG Q L, LI D Y, XU Y, GE H L, LU Q Y. Research progress on design of high entropy oxides and their applications in lithium-ion batteries[J]. Chinese J. Inorg. Chem., 2023, 39: 2241-2255
18. [18]
  WANG X, KANG Q, YAN L, MA T. Understanding the key role of cocktail effect in high-entropy materials for Li-ion and Na-ion batteries[J]. Energy Storage Mater., 2026, 84: 104819 doi: 10.1016/j.ensm.2025.104819
19. [19]
  DUAN L, ZHANG Y, TANG H, LIAO J, ZHOU G, ZHOU X. Recent advances in high-entropy layered oxide cathode materials for alkali metal-ion batteries[J]. Adv. Mater., 2025, 37, 2411426 doi: 10.1002/adma.202411426
20. [20]
  WEN H, KANG W B, LIU X G, LI W J, ZHANG L P, ZHANG C H. Two-phase interface hydrothermal synthesis of binder-free SnS₂/ graphene flexible paper electrodes for high-performance Li-ion batteries[J]. RSC Adv., 2019, 9: 23607-23613 doi: 10.1039/C9RA03397A
21. [21]
  SHUANG W, XU J J, CHEN F Y, WU Y J, YANG L, BAI Z Y. High mixing entropy of MnFeCoNiCu-S to drive high performance sodium storage[J]. Mater. Horizons, 2025, 12(16): 6209-6216 doi: 10.1039/D5MH00163C
22. [22]
  YE J B, CHEN T, CHEN Q N, CHEN W X, YU Z T, XU S R. Facile hydrothermal synthesis of SnCoS₄/graphene composites with excellent electrochemical performance for reversible lithium ion storage[J]. J. Mater. Chem. A, 2016, 4: 13194-13202 doi: 10.1039/C6TA04196E
23. [23]
  ZHOU C, MA X T, LIU G J, DING J J, LV Z Q, LI X, ZHANG B B, YANG Z L, XU W L. Three-dimensional interwoven CoS₂/reduced graphene oxide/carbon nanotubes composite as anode materials for high-performance lithium-ion batteries[J]. J. Alloy. Compd., 2024, 972: 172800 doi: 10.1016/j.jallcom.2023.172800
24. [24]
  ZHAO J, ZHANG Y, CHEN X, SUN G, YANG X, ZENG Y, TIAN R Y, DU F. Entropy-change driven highly reversible sodium storage for conversion-type sulfide[J]. Adv. Funct. Mater., 2022, 32: 2206531 doi: 10.1002/adfm.202206531
25. [25]
  ZHANG S, ZUO W, FU X, LI J, ZHANG Q, YANG W, CHEN H, ZHANG J, XIAO X, AMINE K, SUN S G, FU F, YE M, XU G L. High-entropy sulfoselenide as negative electrodes with fast kinetics and high stability for sodium-ion batteries[J]. Nat. Commun., 2025, 16: 4052 doi: 10.1038/s41467-025-59078-6
1. [1]
  Shan Zhao , Xu Liu , Haotian Guo , Zonglin Liu , Pengfei Wang , Jie Shu , Tingfeng Yi . Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries. Acta Physico-Chimica Sinica, 2026, 42(1): 100129-0. doi: 10.1016/j.actphy.2025.100129
2. [2]
  Jingyu Cai , Xiaoyu Miao , Yulai Zhao , Longqiang Xiao . Exploratory Teaching Experiment Design of FeOOH-RGO Aerogel for Photocatalytic Benzene to Phenol. University Chemistry, 2024, 39(4): 169-177. doi: 10.3866/PKU.DXHX202311028
3. [3]
  Ruolin CHENG , Yue WANG , Xiyao NIU , Huagen LIANG , Ling LIU , Shijian LU . Efficient photothermal catalytic CO₂ cycloaddition over W₁₈O₄₉/rGO composites. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1276-1284. doi: 10.11862/CJIC.20240424
4. [4]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
5. [5]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
6. [6]
  Wentao Xu , Xuyan Mo , Yang Zhou , Zuxian Weng , Kunling Mo , Yanhua Wu , Xinlin Jiang , Dan Li , Tangqi Lan , Huan Wen , Fuqin Zheng , Youjun Fan , Wei Chen . Bimetal Leaching Induced Reconstruction of Water Oxidation Electrocatalyst for Enhanced Activity and Stability. Acta Physico-Chimica Sinica, 2024, 40(8): 2308003-0. doi: 10.3866/PKU.WHXB202308003
7. [7]
  Yue Zhang , Bao Li , Lixin Wu . GO-Assisted Supramolecular Framework Membrane for High-Performance Separation of Nanosized Oil-in-Water Emulsions. Acta Physico-Chimica Sinica, 2024, 40(5): 2305038-0. doi: 10.3866/PKU.WHXB202305038
8. [8]
  Yunting Shang , Yue Dai , Jianxin Zhang , Nan Zhu , Yan Su . Something about RGO (Reduced Graphene Oxide). University Chemistry, 2024, 39(9): 273-278. doi: 10.3866/PKU.DXHX202306050
9. [9]
  Rongzhan LOU , Qiaoling KANG , Zhenchao BAI , Dongyun LI , Yang XU , Rui WANG , Qingyi LU . Research progress of sodium ion high entropy layered oxide cathode. Chinese Journal of Inorganic Chemistry, 2025, 41(12): 2411-2428. doi: 10.11862/CJIC.20250142
10. [10]
  Chaolin Mi , Yuying Qin , Xinli Huang , Yijie Luo , Zhiwei Zhang , Chengxiang Wang , Yuanchang Shi , Longwei Yin , Rutao Wang . Galvanic Replacement Synthesis of Graphene Coupled Amorphous Antimony Nanoparticles for High-Performance Sodium-Ion Capacitor. Acta Physico-Chimica Sinica, 2024, 40(5): 2306011-0. doi: 10.3866/PKU.WHXB202306011
11. [11]
  Yuying JIANG , Jia LUO , Zhan GAO . Development status and prospects of solid oxide cell high entropy electrode catalysts. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1719-1730. doi: 10.11862/CJIC.20250124
12. [12]
  Xin Han , Zhihao Cheng , Jinfeng Zhang , Jie Liu , Cheng Zhong , Wenbin Hu . Design of Amorphous High-Entropy FeCoCrMnBS (Oxy) Hydroxides for Boosting Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2025, 41(4): 100033-0. doi: 10.3866/PKU.WHXB202404023
13. [13]
  Zeyu XU , Tongzhou LU , Haibo SHAO , Jianming WANG . Preparation and electrochemical lithium storage performance of porous silicon microsphere composite with metal modification and carbon coating. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1995-2008. doi: 10.11862/CJIC.20240164
14. [14]
  Kai PENG , Xinyi ZHAO , Zixi CHEN , Xuhai ZHANG , Yuqiao ZENG , Jianqing JIANG . Progress in the application of high-entropy alloys and high-entropy ceramics in water electrolysis. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1257-1275. doi: 10.11862/CJIC.20240454
15. [15]
  Xiaofei Liu , He Wang , Li Tao , Weimin Ren , Xiaobing Lu , Wenzhen Zhang . Electrocarboxylation of Benzylic Phosphates and Phosphinates with Carbon Dioxide. Acta Physico-Chimica Sinica, 2024, 40(9): 2307008-0. doi: 10.3866/PKU.WHXB202307008
16. [16]
  Ji-Quan Liu , Huilin Guo , Ying Yang , Xiaohui Guo . Calculation and Discussion of Electrode Potentials in Redox Reactions of Water. University Chemistry, 2024, 39(8): 351-358. doi: 10.3866/PKU.DXHX202401031
17. [17]
  Linbao Zhang , Weisi Guo , Shuwen Wang , Ran Song , Ming Li . Electrochemical Oxidation of Sulfides to Sulfoxides. University Chemistry, 2024, 39(11): 204-209. doi: 10.3866/PKU.DXHX202401009
18. [18]
  Shiqian WEI , Xinyu TIAN , Hong LIU , Maoxia CHEN , Fan TANG , Qiang FAN , Weifeng FAN , Yu HU . Oxygen reduction reaction/oxygen evolution reaction catalytic performances of different active sites on nitrogen-doped graphene loaded with iron single atoms. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1776-1788. doi: 10.11862/CJIC.20250102
19. [19]
  Zeyu XU , Anlei DANG , Bihua DENG , Xiaoxin ZUO , Yu LU , Ping YANG , Wenzhu YIN . Evaluation of the efficacy of graphene oxide quantum dots as an ovalbumin delivery platform and adjuvant for immune enhancement. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1065-1078. doi: 10.11862/CJIC.20240099
20. [20]
  Zhaoyu Wen , Na Han , Yanguang Li . Recent Progress towards the Production of H₂O₂ by Electrochemical Two-Electron Oxygen Reduction Reaction. Acta Physico-Chimica Sinica, 2024, 40(2): 2304001-0. doi: 10.3866/PKU.WHXB202304001

Get Citation

PDF

XML

Metrics

PDF Downloads(14)
Abstract views(240)
HTML views(35)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Synthesis and electrochemical lithium storage performance of high-entropy NiCoSnZnFeSx and reduced graphene oxide composite

Metrics

通讯作者: 陈斌, bchen63@163.com

Synthesis and electrochemical lithium storage performance of high-entropy NiCoSnZnFeS_x and reduced graphene oxide composite