Fabrication and electrochemical properties of hollow cage-like nickel cobalt layered hydroxides with porous structure

Yang Wen; Ding Qian-Yao; Zhai Dong-Mei; Bo Kai-Wen; Feng Yan-Yan; Wen Jie; He Fang

doi:10.7498/aps.71.20211100

Abstract

Supercapacitors have attracted extensive attention in various storage devices due to their high power density, long life and friendly environment. Hence, improving the energy storage performances of electrode materials are of great significance for supercapacitors. Functional materials with specific nanostructures, as energy storage materials, can display excellent electrochemical performances, for they will provide rich electrochemically active sites, high specific surface area and enhance electrolyte contact area. Consequently, hollow cage-like nickel cobalt layered hydroxides (NiCo-LDH) are prepared via nitrate etching of ZIF-67 nanocrystals, and investigated as electrode materials of supercapacitor. The morphology, structure and electrochemical properties of the obtained materials are investigated by X-ray diffraction, scanning electron microscope, transmission electron microscope, N ₂ adsorption/desorption and a series of electrochemical tests (including cyclic voltammetry, galvanostatic charge and discharge and AC impedance). The results show that the NiCo-LDH samples assembled by nanosheets present a porous structure with hollow cages and high specific area surfaces, which conduces to increasing the electroactive sites, enhancing the contact between the electrolyte and the electrode material, and thus significantly improving the electrochemical performance of the materials. With the mass ratio of nickel to cobalt salt being 1∶1, the specific capacitance of Ni ₁Co ₁-LDH is 801 F·g ^–1 at a current density of 0.5 A·g ^–1, and a specific capacitance of 582 F·g ^–1 can still be maintained at a high current density of 10 A·g ^–1. Moreover, the specific capacitance retention of Ni ₁Co ₁-LDH is 100.2% after 2000 cycles at a current density of 15 A·g ^–1, displaying good electrochemical performance and great potential in supercapacitor applications.

Keywords:

Authors and contacts

1.
Guangxi Key Laboratory of Electrochemical and Magneto-chemical Functional Materials, College of Chemistry and Bioengineering, Guilin University of Technology, Guilin 541004, China
2.
College of Chemistry and Bioengineering, Guilin University of Technology, Guilin 541004, China
3.
College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China

Corresponding author: Feng Yan-Yan, feng1988glut@163.com

Funds: Project supported by the Natural Science Foundation of Guangxi Zhuang Autonomous Region, China (Grant Nos. 2017GXNSFBA198124, 2017GXNSFBA198193), the National Natural Science Foundation of China (Grant No. 21606058), and the Guangxi Key Laboratory of Electrochemical and Magneto-chemical Functional Materials, China (Grant No. EMFM20211101)

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References

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[5]	Cai Z X, Wang Z L, Kim J, Yamauchi Y 2019 Adv. Mater. 31 1804903 Google Scholar
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[8]	Xiao P W, Meng Q H, Zhao L, Li J J, Wei Z X, Han B H 2017 Mater. Des. 129 164 Google Scholar
[9]	Liu D, Du P C, Wei W L, Wang H X, Liu P 2018 J. Colloid. Interface Sci. 513 295 Google Scholar
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[15]	Xuan X Y, Qian M, Han L, Wan L J, Li Y Q, Lu T, Pan L K, Niu Y P, Gong S Q 2019 Electrochim. Acta 321 134710 Google Scholar
[16]	冯艳艳, 黄宏斌, 张心桔, 易亚军, 杨文 2017 66 248202 Google Scholar Feng Y Y, Huang H b, Zhang X J, Yi Y J, Yang W 2017 Acta Phys. Sin. 66 248202 Google Scholar
[17]	Huang Q, Liu K Y, He F, Zhang S R, Xie Q L, Chen C 2017 Trans. Nonferrous Met. Soc. 27 1804 Google Scholar
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[36]	Wang D, Tian L Y, Li D W, Xu Y, Wei Q F 2020 J. Electroanal. Chem. 873 114377 Google Scholar
[37]	Liu Y X, Wang Y Z, Shi C J, Chen Y J, Li D, He Z F, Wang C, Guo L, Ma J M 2020 Carbon 165 129 Google Scholar
[38]	Tahir M. U, Arshad H, Xie W Y, Wang X L, Nawaz M, Yang C, Su X T 2020 Appl. Surf. Sci. 529 147073 Google Scholar
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[40]	Zang Y, Luo H, Zhang H, Xue H G 2021 ACS Appl. Energy Mater. 4 1189 Google Scholar
[41]	Jiang Z, Li Z P, Qin Z H, Sun H Y, Jiao X L, Chen D R 2013 Nanoscale 5 11770 Google Scholar
[42]	Liu L L, Fang L, Wu F, Hu J, Zhang S F, Luo H J, Hu B S, Zhou M 2020 J. Alloys Compd. 824 153929 Google Scholar
[43]	Yang F, Chu J, Cheng Y P, Gong J F, Wang X Q, Xiong S X 2021 Chem. Res. Chin. U. 37 772 Google Scholar
[44]	Wan H Z, Li L, Xu Y, Tan Q Y, Liu X, Zhang J, Wang H B, Wang H 2018 Nanotechnology 29 194003 Google Scholar
[45]	Li Y L, Li Q, Zhao S H, Chen C, Zhou J J, Tao K, Han L 2018 ChemistrySelect 3 13596 Google Scholar
[46]	Lv Z J, Zhong Q, Bu Y F 2018 Adv. Mater. Interfaces 5 1800438 Google Scholar
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Cited By

图 1 中空笼状NiCo-LDH的制备示意图

Figure 1. Schematic illustration of the preparation of hollow cage-like NiCo-LDH.

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图 2 样品的X射线衍射谱图

Figure 2. XRD patterns of the samples.

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图 3 样品的扫描电镜图　(a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH

Figure 3. SEM images of the samples: (a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH.

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图 4 样品Ni ₁Co ₁-LDH的能谱分析　(a) 总图; (b) Co元素; (c) Ni元素

Figure 4. EDS profiles of the sample Ni ₁Co ₁-LDH: (a) Total mapping; (b) Co element; (c) Ni element.

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图 5 样品的透射电镜图　(a) ZIF-67; (b) Ni ₀Co ₁-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₂Co ₁-LDH; (f) Ni ₁Co ₀-LDH

Figure 5. TEM images of the samples: (a) ZIF-67; (b) Ni ₀Co ₁-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₂Co ₁-LDH; (f) Ni ₁Co ₀-LDH.

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图 6 样品的(a)氮气吸附/脱附等温线和(b)孔径分布图

Figure 6. (a) N ₂ adsorption/desorption isotherms and (b) pore size distributions of the samples.

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图 7 样品在不同扫描速度下的循环伏安曲线　(a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH

Figure 7. CV curves of the samples at different scan rates: (a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH.

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图 8 样品在不同电流密度下的恒电流充放电曲线　(a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH

Figure 8. GCD curves of the samples at various current densities: (a) Ni ₀Co ₁-LDH; (b) Ni ₁Co ₂-LDH; (c) Ni ₁Co ₁-LDH; (d) Ni ₂Co ₁-LDH; (e) Ni ₁Co ₀-LDH.

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图 9 样品在不同电流密度下的(a)比电容和(b)电容保留率

Figure 9. (a) Specific capacitances and (b) capacitance retentions of the samples under various current densities.

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图 10 样品在电流密度为15 A·g ^–1下的循环稳定性能

Figure 10. Cyclic performance of the samples at the current density of 15 A·g ^–1.

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图 11 样品的(a), (b)Nyquist曲线和(c)高频区Nyquist曲线的放大图

Figure 11. (a), (b) Nyquist curves and (c) the enlarged curves at the high frequency range of the samples.

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表 1 样品的孔结构参数

Table 1. Pore structure parameters of the samples.

Sample	Ni/Co molar ratio	BET specific surface area/m ²·g ^–1	Pore volume (meso)/(cm ³·g ^–1)	Average pore width/nm	Average pore width (meso)/nm
Ni ₀Co ₁-LDH	0	81.4	0.443	18.2	17.5
Ni ₁Co ₂-LDH	0.18	112.7	0.600	17.9	16.5
Ni ₁Co ₁-LDH	0.39	182.6	0.954	17.9	16.3
Ni ₂Co ₁-LDH	0.45	194.3	0.973	17.8	15.4
Ni ₁Co ₀-LDH	2.37	233.3	0.913	13.2	11.5

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表 2 NiCo-LDH基电极材料的比电容值比较

Table 2. Comparison of specific capacitances of various NiCo-LDH based electrodes materials.

Sample	Electrolyte	Specific capacitance/(F·g ^–1)	Reference
Ni ₂Co ₁-LDH	2 M KOH	963 (0.5 A·g ^–1)	本文
MnO ₂-2/NiCo-LDH/CC	1 M NaSO ₄	312 (0.2 A·g ^–1)	[ 42]
NiCo@BC	6 M KOH	606.4 (0.5 A·g ^–1)	[ 43]
Ni-Co LDH/NiNw	6 M KOH	466.6 (0.125 A·g ^–1)	[ 44]
NiCo LDH@Ni-CAT	1 M KOH	882 (1 A·g ^–1)	[ 45]
NCLDH@CNTs	6 M KOH	916.8 (1 A·g ^–1)	[ 46]
10%Ce-NiCo-LDH/CNT	1 M KOH	187.2 (1 A·g ^–1)	[ 47]
MnO ₂/NiCo-LDH	6 M KOH	555.6 (1 A·g ^–1)	[ 48]

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map

[1]	González A, Goikolea E, Barrena J A, Mysyk R 2016 Renewable Sustainable Energy Rev. 58 1189 Google Scholar
[2]	Zha D S, Sun H H, Fu Y S, Ouyang X P, Wang X 2017 Electrochim. Acta 236 18 Google Scholar
[3]	Zhang L J, Hui K N, Hui S K, Lee H 2016 J. Power Sources 318 76 Google Scholar
[4]	Wang H T, Jin C, Liu Y N, Kang X H, Bian S W, Zhu Quan 2018 Electrochim. Acta 283 1789 Google Scholar
[5]	Cai Z X, Wang Z L, Kim J, Yamauchi Y 2019 Adv. Mater. 31 1804903 Google Scholar
[6]	Li L, Liu X, Liu C, Wang H Z, Zhang J, Liang P, Wang H B, Wang H 2018 Electrochim. Acta 259 303 Google Scholar
[7]	张诚, 邓明森, 蔡绍洪 2017 66 128201 Google Scholar Zang C, Deng M S, Cai S H 2017 Acta Phys. Sin. 66 128201 Google Scholar
[8]	Xiao P W, Meng Q H, Zhao L, Li J J, Wei Z X, Han B H 2017 Mater. Des. 129 164 Google Scholar
[9]	Liu D, Du P C, Wei W L, Wang H X, Liu P 2018 J. Colloid. Interface Sci. 513 295 Google Scholar
[10]	冯艳艳, 李彦杰, 杨文, 牛潇迪 2020 化工进展 39 2734 Feng Y Y, Li Y J, Yang W, Niu X D 2020 Chem. Ind. Eng. Prog. 39 2734
[11]	Ryu I, Yang M H, Kwon H, Park H K, Do Y R, Lee S B, Yim S 2014 Langmuir 30 1704 Google Scholar
[12]	Shi P P, Li L, Hua L, Qian Q Q, Wang P F, Zhou J Y, Sun G Z, Huang W 2017 ACS Nano 11 444 Google Scholar
[13]	Shen K W, Ran F, Zhang X X, Liu C, Wang N J, Niu X Q, Liu Y, Zhang D J, Kong L B, Kang L, Chen S W 2015 Synth. Met. 209 369 Google Scholar
[14]	Nanwani A, Deshmukh K A, Sivaraman P, Peshwe D R, Sharma I, Dhoble S J, Swart H C, Deshmukh A D, Gupta B K 2019 Npj 2 D Mater. Appl. 3 1 Google Scholar
[15]	Xuan X Y, Qian M, Han L, Wan L J, Li Y Q, Lu T, Pan L K, Niu Y P, Gong S Q 2019 Electrochim. Acta 321 134710 Google Scholar
[16]	冯艳艳, 黄宏斌, 张心桔, 易亚军, 杨文 2017 66 248202 Google Scholar Feng Y Y, Huang H b, Zhang X J, Yi Y J, Yang W 2017 Acta Phys. Sin. 66 248202 Google Scholar
[17]	Huang Q, Liu K Y, He F, Zhang S R, Xie Q L, Chen C 2017 Trans. Nonferrous Met. Soc. 27 1804 Google Scholar
[18]	Huang W G, Zhang A T, Li X R, Tian J M, Yue L J, Cui L, Zheng R K, Wei D, Liu J Q 2019 J. Power Sources 440 227123 Google Scholar
[19]	Xu J, Ma C J, Cao J Y, Chen Z D 2017 Dalton Trans. 46 3276 Google Scholar
[20]	Xiao Z Y, Bao Y X, Li Z J, Huai X D, Wang M H, Liu P, Wang L 2019 ACS Appl. Energy Mater. 2 1086 Google Scholar
[21]	Yang Z, Wang X M, Zhang H, Yan S H, Zhang C, Liu S X 2019 ChemElectroChem 6 4456 Google Scholar
[22]	Cheng C, Wei C Z, He Y Y, Liu L Y, Hu J Y, Du W M 2021 J. Energy Storage 33 102105 Google Scholar
[23]	Li X Y, Yu L, Wang G L, Wan G P, Peng X G, Wang K, Wang G Z 2017 Electrochim. Acta 255 15 Google Scholar
[24]	Xiao Z Y, Mei Y J, Yuan S, Mei H, Xu B, Bao Y X, Fan L L, Kang W P, Dai F N, Wang R, Wang L, Hu S Q, Sun D F, Zhou H C 2019 ACS Nano 13 7024 Google Scholar
[25]	Xu Y Q, Hou S J, Yang G, Wang X J, Lu T, Pan L K 2018 Electrochim. Acta 285 192 Google Scholar
[26]	Yu L, Hu H, Wu H B, Lou X W 2017 Adv. Mater. 29 1604563 Google Scholar
[27]	Hu H, Guan B Y, Xia B Y, Lou X W 2015 J. Am. Chem. Soc. 137 5590 Google Scholar
[28]	Liu D, Wan J W, Pang G S, Tang Z Y 2019 Adv. Mater. 31 1803291 Google Scholar
[29]	Rashti A, Lu X, Dobson A, Hassani E, Feyzbar-Khalkhali-Nejad F, He K, Oh T S 2021 ACS Appl. Energy Mater. 4 1537 Google Scholar
[30]	Liu K, Yu M L, Wang H Y, Wang J, Liu W P, Hoffmann M R 2019 Environ. Sci. Technol. 53 6474 Google Scholar
[31]	Zhu Y Y, Zhou Y N, Zhang X, Sun Z G, Jiao C Q 2021 Adv. Opt. Mater. 9 2001889 Google Scholar
[32]	Li R, Che R, Liu Q, Su S Z, Li Z S, Zhang H S, Liu J Y, Liu L H, Wang J 2017 J. Hazard. Mater. 338 167 Google Scholar
[33]	Song X K, Jiang Y, Cheng F, Earnshaw J, Na J, Li X P, Yamauchi Y 2021 Small 17 2004142 Google Scholar
[34]	Hou S Y, Lian Y, Bai Y Q, Zhou Q P, Ban C L, Wang Z F, Zhao J, Zhang H H 2020 Electrochim. Acta 341 136053 Google Scholar
[35]	Wu H, Zhang Y N, Yuan W Y, Zhao Y X, Luo S H, Yuan X W, Zheng L X, Cheng L F 2018 J. Mater. Chem. A 6 16617 Google Scholar
[36]	Wang D, Tian L Y, Li D W, Xu Y, Wei Q F 2020 J. Electroanal. Chem. 873 114377 Google Scholar
[37]	Liu Y X, Wang Y Z, Shi C J, Chen Y J, Li D, He Z F, Wang C, Guo L, Ma J M 2020 Carbon 165 129 Google Scholar
[38]	Tahir M. U, Arshad H, Xie W Y, Wang X L, Nawaz M, Yang C, Su X T 2020 Appl. Surf. Sci. 529 147073 Google Scholar
[39]	Chu H L, Zhu Y, Fang T T, Hua J Q, Qiu S J, Liu H D, Qin L Y, Wei Q H, Zou Y J, Xiang C L, Xu F, Sun L X 2020 Sustainable Energy Fuel 4 337 Google Scholar
[40]	Zang Y, Luo H, Zhang H, Xue H G 2021 ACS Appl. Energy Mater. 4 1189 Google Scholar
[41]	Jiang Z, Li Z P, Qin Z H, Sun H Y, Jiao X L, Chen D R 2013 Nanoscale 5 11770 Google Scholar
[42]	Liu L L, Fang L, Wu F, Hu J, Zhang S F, Luo H J, Hu B S, Zhou M 2020 J. Alloys Compd. 824 153929 Google Scholar
[43]	Yang F, Chu J, Cheng Y P, Gong J F, Wang X Q, Xiong S X 2021 Chem. Res. Chin. U. 37 772 Google Scholar
[44]	Wan H Z, Li L, Xu Y, Tan Q Y, Liu X, Zhang J, Wang H B, Wang H 2018 Nanotechnology 29 194003 Google Scholar
[45]	Li Y L, Li Q, Zhao S H, Chen C, Zhou J J, Tao K, Han L 2018 ChemistrySelect 3 13596 Google Scholar
[46]	Lv Z J, Zhong Q, Bu Y F 2018 Adv. Mater. Interfaces 5 1800438 Google Scholar
[47]	DinariI M, Allami H, Momeni M M 2020 Energy Fuel. 35 1831
[48]	Wu S H, Zhang J Z, Sun C, Chen J S 2020 J. Inorg. Organomet. Polym. 30 3179 Google Scholar

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Vol. 71, Issue 1 - 2022-01-05

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