J. Semicond. > 2023, Volume 44 > Issue 4 > 041601, doi: 10.1088/1674-4926/44/4/041601
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Layered double hydroxides as electrode materials for flexible energy storage devices

Qifeng Lin1, 3 and Lili Wang1, 2,

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 Corresponding author: Lili Wang, liliwang@semi.ac.cn

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Abstract: To prevent and mitigate environmental degradation, high-performance and cost-effective electrochemical flexible energy storage systems need to be urgently developed. This demand has led to an increase in research on electrode materials for high-capacity flexible supercapacitors and secondary batteries, which have greatly aided the development of contemporary digital communications and electric vehicles. The use of layered double hydroxides (LDHs) as electrode materials has shown productive results over the last decade, owing to their easy production, versatile composition, low cost, and excellent physicochemical features. This review highlights the distinctive 2D sheet-like structures and electrochemical characteristics of LDH materials, as well as current developments in their fabrication strategies for expanding the application scope of LDHs as electrode materials for flexible supercapacitors and alkali metal (Li, Na, K) ion batteries.

Key words: layered double hydroxide, flexible energy storage devices, structural designs, electrochemical performances



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Fig. 1.  (Color online) General composition of LDHs[25]. Copyright 2021 , Elsevier Ltd.

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Fig. 2.  (Color online) SEM images of (a) H-NiCo LDH powder, (b) ZIF-67@ACC, and (c) H-NiCo LDH@ACC. (d, f) Capacity comparison curve of H-NiCo LDH@ACC and ACF. (e) Optical image of flexible H-NiCo LDH@ACC//AC devices[44]. Copyright 2019, Elsevier Ltd.

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Fig. 3.  (Color online) (a) Illustration of flexible Ni–Co LDH@rGO devices. (b) SEM image of 3D Ni–Co LDH@rGO. (c) Charge-discharge curves at different current densities and (d) Ragone plot for the Ni–Co LDH@// crumpled rGO device. (e) Cycle life and Coulombic efficiency curves for the hybrid device. (f–h) Application of flexible Ni–Co LDH@rGO devices[47]. Copyright 2020, Elsevier Ltd.

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Fig. 4.  (Color online) (a) Synthesis schematic of NiCo-OH/ZnO-NR/CNT-yarn fiber. (b) Schematic diagrams and photographs of the bending angles of a symmetric two-electrode supercapacitor device composed of two NiCo-OH/ZnONR/CNT-yarns at each bending angle. (c) CV curves of the symmetric supercapacitor at different bending angles and (d) capacitance retention after 1000 cycles at a bending angle of 150° and the scan rate of 100 mV/s[51]. Copyright 2020, Elsevier Ltd.

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Fig. 5.  (Color online) (a) Synthesis sequence diagram of MLDH@PAC. (b) Long-term coulombic efficiency and specific capacity in alternating bend-flat state[58]. Copyright 2019, American Chemical Society.

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Fig. 6.  (Color online) The (a) flow chart, (b) SEM and (c) TEM image of the GAL film. (d) Photographic images of the GAL film and ASFC device. (e) Photographic image, (f) CV and (g) GCD curves of GAL//GAL AFSC device at various bending angles[10]. Copyright 2022, Elsevier Ltd.

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Fig. 7.  (Color online) (a) Elemental mapping image of Co–Mn LDH. (b) Comparison of GCD curves of various devices. (c) Optical image of the flexible energy storage devices under bent angles. CV curves of flexible device under (d) 0–180° and (e) –30 to –180°. (f) Optical image of a flexible device unit application[63]. Copyright 2020, Elsevier Ltd.

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Fig. 8.  (Color online) (a) Schematic illustration of the CC@NiCo2-OH and CC@NiCo2AlX-LDH grown on carbon cloth. (b) Photographs of FASC bent at 0°, 45°, 90°, 180°. (c) GCD curves and (d) specific capacitance retention of the FASC at a current density of 2 A/g. (e) Comparison energy density of various energy storage device[72]. Copyright 2019, Wiley-VCH Verlag GmbH&Co. KGaA, Weinheim.

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Fig. 9.  (Color online) (a) Schematic illustration of the synthesis process of NSPCs. (b) 120-cycle curves at different current density of 0.5 and 6 C. (c) Rate performance curves of NSPCs-800[81]. Copyright 2016, The Royal Society of Chemistry.

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Fig. 10.  (Color online) (a) Schematic diagram of TMOs@MXene hollow polyhedron. (b) TEM image of TMOs@MXene hollow polyhedron. (c) Rate performance of pristine Ti3C2Tx, CoO/Co2Mo3O8 and CoO/Co2Mo3O8@MXene anodes. (d) CoO/Co2Mo3O8@MXene's 1200 cycle stability curve under 2 A/g[76]. Copyright 2019, Wiley-VCH Verlag GmbH&Co. KGaA, Weinheim.

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Fig. 11.  (Color online) (a) The charge-discharge capacity curve at the 1st, 2nd, and 5th laps and (b) cycling performance of CoFe-NO3–-LDH at 1 A/g. The (c) side view and (d) top view of Na migration model diagram. (e) The diffusion barrier profiles for Na migration along the path TC→TE→TC[87]. Copyright 2019, The Royal Society of Chemistry.

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Fig. 12.  (Color online) (a) The schematic illustration of box-in-box structure of Co/(NiCo)Se2. (b) Tafel plots, (c) cycle stability and (d) rate performance of the Co/(NiCo)Se2 nanocubes[77]. Copyright 2017, The Royal Society of Chemistry.

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Fig. 13.  (Color online) (a) Fabrication illustration of bulk TiO2 and TCNS. (b) TEM images of Zn–Ti LDH, (c–f) ultrahigh stability and a specific capacity of Zn–Ti LDH@PV[88]. Copyright 2021, Elsevier Ltd.

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Fig. 14.  (Color online) SEM images of (a) LDH, (b) LDH-S and (c) CDs@LDH-S. (d) Cycling performances of CDs and CDs@LDH-S at 1 A/g. (e) Rate performance at different current density of LDH, LDH-S and CDs@LDH-S. Cycling performance at (f) 0.1 A/g and (g) 0.5 A/g of LDH, LDH-S and CDs@LDH-S[94]. Copyright 2021, Elsevier Ltd.

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Table 1.   Performance comparison of LDH-based electrodes for supercapacitors.

MaterialElectrolyteTest methodSpecific capacitance/
current density		Capacitance retention (Cycle/current density)Energy density/
Power density		Ref.
Mn-doped Ni–Co LDH@polyaniline-
derived carbon		6 M KOHAll-solid-state flexible asymmetric supercapacitor1282.06 C/g/
1 A/g		82.66% (8000th/10 A/g)78.9 W·h/kg/
1.55 kW/kg		[58]
Hollow Ni–Co LDH@
acidified carbon cloth		2 M KOHFlexible free-standing asymmetric supercapacitor1377 mC/cm2/
1 mA/cm2		70% (10000th/
80 mA/cm2)		0.0708 mW·h/cm2/
0.7 mW/cm2		[44]
Ni–Co LDH@rGO3 M KOHAsymmetric supercapacitor2640 F/g/
1 A/g		80.2% (4000th)58.4 W·h/kg/
3.73 kW/kg		[47]
NiCo-OH/ZnO-NR/
CNT-yarn		1 M LiOHFlexible symmetric supercapacitor1278 F/g60.5% (7000th/
30 Ma/cm2)		1.38 μW·h/cm2/
647 μW/cm2		[51]
rGO@Ag nanowire/
Ni-Al LDH		6 M KOHAll-solid-state flexible asymmetric supercapacitor127.2 F/g/
1 A/g		83.2% (10000th/1 A/g)35.75 mW·h/cm3/
1.01 W/cm3		[10]
Ni–Fe LDH@rGO@NF2 M KOHFlexible asymmetric supercapacitor1462.5 F/g/
5 A/g		64.7% (2000th/15 A/g)17.71 W·h/kg/
348.49 W/kg		[59]
Co-Al LDH@Ni-Co
LDH//CC		6 M KOHFlexible quasisolid-state asymmetric supercapacitor2633. 6 F/g/
1 A/g		92.5% (5000th/4 A/g)57.8 W·h/kg/
0.81 kW/kg		[64]
Co–Mn LDH@MnO23 M KOHFlexible asymmetric supercapacitor2325.01 F/g/
1 A/g		95% (10000th/
30 mA/cm2)		59.73 W·h/kg/
1000.09 W/kg		[63]
CC@NiCo2Al LDH1 M KOHFlexible asymmetric supercapacitor1137 F/g/
0.5 A/g		91.2% (15000th/5 A/g)44 W·h/kg/
462 W/kg		[72]
Zn–Mg–Al LDH@
Fe2O3/3D HPCNF		3 M KOHAll-solid-state symmetric supercapacior3437 F/cm2/
1 mA/cm2		106.5% (40000th/
50 mA/cm2)		11.62 mW·h/cm3/
9.999 mW/cm3		[73]
DownLoad: CSV

Table 2.   Electrochemical performances of various LDHs-based electrode materials in AIBs.

MaterialBattery TypeCycling stability (cycle)/
Current density		Rate performanceInitial coulombic efficiencyRef.
ZnO/ZnAl2O4LIBs1275 mA·h/g (10th)/0.2 A/g––[80]
Nitrogen and sulfur co-doped porous carbonLIBs1175 mA·h/g (120th)/0.5 C360 mA·h/g at 30 C–[81]
CoO/Co2Mo3O8@MXeneLIBs545 mA·h/g (1200th)/2 A/g386.1 mA·h/g at 5 A/g71%[76]
Multiphase Mn-doped Ni sulfides@rGOLIBs206.1 mA·h/g (50th)/0.1 A/g103.6 mA·h/g at 1 A/g68%[82]
Co/(Ni, Co)Se2SIBs497 mA·h/g (80th)/0.2 A/g456 mA·h/g at 5 A/g80%[77]
Multiphase Mn-doped Ni sufides@rGOSIBs206.1 mA·h/g (2000th)/0.5 A/g229.2 mA·h/g at 5 A/g–[75]
CoFe-NO3--LDHSIBs209 mA·h/g (200th)/1 A/g228 mA·h/g at at 2 A/g–[87]
TiO2 nanoparticles@CNSSIBs196.7 mA·h/g (2000th)/2 A/g197.2 mA·h/g at 10 A/g41%[88]
MgFe-LDHKIBs371.6 mA·h/g (300th)/0.1 A/g144.5 mA·h/g at 10 A/g88%[94]
CDs@LDH-SKIBs188 mA·h/g (8000th)/1 A/g172 mA·h/g at 5 A/g–[95]
DownLoad: CSV
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Zhao C, Wang Z J, Shu D J, et al. Preface to the special issue on challenges and possibilities of energy storage. J Semicond, 2020, 41, 090101 doi: 10.1088/1674-4926/41/9/090101

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    Received: 15 November 2022 Revised: 30 November 2022 Online: Accepted Manuscript: 09 February 2023Uncorrected proof: 10 February 2023Published: 10 April 2023

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      Article Navigation >  Journal of Semiconductors  > 2023  >  44(4): 041601
      Qifeng Lin, Lili Wang. Layered double hydroxides as electrode materials for flexible energy storage devices[J]. Journal of Semiconductors, 2023, 44(4): 041601. doi: 10.1088/1674-4926/44/4/041601 Q F Lin, L L Wang. Layered double hydroxides as electrode materials for flexible energy storage devices[J]. J. Semicond, 2023, 44(4): 041601. doi: 10.1088/1674-4926/44/4/041601Export: BibTex EndNote
      Citation:
      Qifeng Lin, Lili Wang. Layered double hydroxides as electrode materials for flexible energy storage devices[J]. Journal of Semiconductors, 2023, 44(4): 041601. doi: 10.1088/1674-4926/44/4/041601

      Q F Lin, L L Wang. Layered double hydroxides as electrode materials for flexible energy storage devices[J]. J. Semicond, 2023, 44(4): 041601. doi: 10.1088/1674-4926/44/4/041601
      Export: BibTex EndNote
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      Layered double hydroxides as electrode materials for flexible energy storage devices

      doi: 10.1088/1674-4926/44/4/041601
      • 1.

        State Key Laboratory for Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China

      • 2.

        Center of Materials Science and Optoelectronic Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

      • 3.

        State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012, China

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      • Author Bio:

        Qifeng Lin is currently a B.S. candidate at College of Electronic Science and Engineering of Jilin University, Changchun, China. His research interests mainly focus on layered double hydroxides materials-based flexible energy storage devices

        Lili Wang is a professor in the Institute of Semiconductors, Chinese Academy of Sciences, China. She earned her B.S. degree in Chemistry and Ph.D degree in Microelectronics and Solid State Electronics from Jilin University in 2014. Her current research interests focus on the semiconductor multimode intelligent sensing integrated system

      • Corresponding author: liliwang@semi.ac.cn
      • Received Date: 2022-11-15
      • Revised Date: 2022-11-30
        • Available Online: 2023-02-09

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