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Title: Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance

Abstract

For miniaturized capacitive energy storage, volumetric and areal capacitances are more important metrics than gravimetric ones because of the constraints imposed by device volume and chip area. Typically used in commercial supercapacitors, porous carbons, although they provide a stable and reliable performance, lack volumetric performance because of their inherently low density and moderate capacitances. Here we report a high-performing electrode based on conductive hexaaminobenzene (HAB)-derived two-dimensional metal-organic frameworks (MOFs). In addition to possessing a high packing density and hierarchical porous structure, these MOFs also exhibit excellent chemical stability in both acidic and basic aqueous solutions, which is in sharp contrast to conventional MOFs. Submillimetre-thick pellets of HAB MOFs showed high volumetric capacitances up to 760 F cm(-3) and high areal capacitances over 20 F cm(-2). Furthermore, the HAB MOF electrodes exhibited highly reversible redox behaviours and good cycling stability with a capacitance retention of 90% after 12,000 cycles. These promising results demonstrate the potential of using redox-active conductive MOFs in energy-storage applications.

Authors:
 [1]; ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [1];  [3];  [4];  [4];  [4];  [1];  [2];  [5];  [1]
+ Show Author Affiliations
  1. Stanford Univ., CA (United States). Department of Chemical Engineering
  2. Stockholm Univ. (Sweden). Berzelii Centre EXSELENT on Porous Materials, Department of Materials and Environmental Chemistry
  3. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division, Advanced Photon Source
  4. Stanford Univ., CA (United States). Department of Chemical Engineering, SUNCAT Center for Interface Science and Catalysis
  5. Stanford Univ., CA (United States). Department of Materials Science and Engineering
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES); Knut and Alice Wallenberg Foundation; Swedish Research Council (SRC)
OSTI Identifier:
1426494
Alternate Identifier(s):
OSTI ID: 1461332
Grant/Contract Number:  
AC02-76SF00515; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Batteries; Metal-organic frameworks

Citation Formats

Feng, Dawei, Lei, Ting, Lukatskaya, Maria R., Park, Jihye, Huang, Zhehao, Lee, Minah, Shaw, Leo, Chen, Shucheng, Yakovenko, Andrey A., Kulkarni, Ambarish, Xiao, Jianping, Fredrickson, Kurt, Tok, Jeffrey B., Zou, Xiaodong, Cui, Yi, and Bao, Zhenan. Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance. United States: N. p., 2018. Web. doi:10.1038/s41560-017-0044-5.
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Feng, Dawei, Lei, Ting, Lukatskaya, Maria R., Park, Jihye, Huang, Zhehao, Lee, Minah, Shaw, Leo, Chen, Shucheng, Yakovenko, Andrey A., Kulkarni, Ambarish, Xiao, Jianping, Fredrickson, Kurt, Tok, Jeffrey B., Zou, Xiaodong, Cui, Yi, & Bao, Zhenan. Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance. United States. https://doi.org/10.1038/s41560-017-0044-5
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Feng, Dawei, Lei, Ting, Lukatskaya, Maria R., Park, Jihye, Huang, Zhehao, Lee, Minah, Shaw, Leo, Chen, Shucheng, Yakovenko, Andrey A., Kulkarni, Ambarish, Xiao, Jianping, Fredrickson, Kurt, Tok, Jeffrey B., Zou, Xiaodong, Cui, Yi, and Bao, Zhenan. Mon . "Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance". United States. https://doi.org/10.1038/s41560-017-0044-5. https://www.osti.gov/servlets/purl/1426494.
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@article{osti_1426494,
title = {Robust and conductive two-dimensional metal-organic frameworks with exceptionally high volumetric and areal capacitance},
author = {Feng, Dawei and Lei, Ting and Lukatskaya, Maria R. and Park, Jihye and Huang, Zhehao and Lee, Minah and Shaw, Leo and Chen, Shucheng and Yakovenko, Andrey A. and Kulkarni, Ambarish and Xiao, Jianping and Fredrickson, Kurt and Tok, Jeffrey B. and Zou, Xiaodong and Cui, Yi and Bao, Zhenan},
abstractNote = {For miniaturized capacitive energy storage, volumetric and areal capacitances are more important metrics than gravimetric ones because of the constraints imposed by device volume and chip area. Typically used in commercial supercapacitors, porous carbons, although they provide a stable and reliable performance, lack volumetric performance because of their inherently low density and moderate capacitances. Here we report a high-performing electrode based on conductive hexaaminobenzene (HAB)-derived two-dimensional metal-organic frameworks (MOFs). In addition to possessing a high packing density and hierarchical porous structure, these MOFs also exhibit excellent chemical stability in both acidic and basic aqueous solutions, which is in sharp contrast to conventional MOFs. Submillimetre-thick pellets of HAB MOFs showed high volumetric capacitances up to 760 F cm(-3) and high areal capacitances over 20 F cm(-2). Furthermore, the HAB MOF electrodes exhibited highly reversible redox behaviours and good cycling stability with a capacitance retention of 90% after 12,000 cycles. These promising results demonstrate the potential of using redox-active conductive MOFs in energy-storage applications.},
doi = {10.1038/s41560-017-0044-5},
journal = {Nature Energy},
number = 1,
volume = 3,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}
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https://doi.org/10.1038/s41560-017-0044-5
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Figures / Tables:

Fig. 1 Fig. 1: | Synthesis and structural characterization of HAB MOFs. a, Synthesis scheme of Cu- /Ni-HAB MOFs. b, Experimental and Powley fitted PXRD patterns of Cu-HAB. c, 2D GIXD pattern of a Cu-HAB thin film on a Si substrate. d, HR-TEM image of Cu-HAB along [001] that shows a hexagonalmore » pore packing with d100=1.15 nm (a=1.33 nm). Scale bar, 10 nm, Inset: Fourier transform of the image. e, HR-TEM image of the region within the blue square in d, f, Symmetry-imposed and lattice-averaged image calculated from the HR-TEM image. Embedded is the eclipsed structure model of Cu-HAB. Scale bar, 2 nm. g,h, Experimental (g) and simulated (h) electron-diffraction pattern (eclipsed model) of Cu-HAB viewed along [-110]. Scale bar 5 nm-1. Insel (g): the crystal from which the electron-diffraction pattern was taken. Scale bar, 50 nm. i, A space-filling model of the Cu-HAB model. Blue, grey, green and white spheres represent N, C, Ni and H atoms, respectively; a.u.: arbitrary units.« less
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    • DOI: 10.1088/2053-1591/ab5752

    Solid–solid interface growth of conductive metal–organic framework nanowire arrays and their supercapacitor application
    journal, January 2020

    • Du, Xing; Zhang, Jianing; Wang, Huali
    • Materials Chemistry Frontiers, Vol. 4, Issue 1
    • DOI: 10.1039/c9qm00527g

    Sodium-coupled electron transfer reactivity of metal–organic frameworks containing titanium clusters: the importance of cations in redox chemistry
    journal, January 2019

    • Saouma, Caroline T.; Tsou, Chih-Chin; Richard, Sarah
    • Chemical Science, Vol. 10, Issue 5
    • DOI: 10.1039/c8sc04138e

    Ultrathin two-dimensional π–d conjugated coordination polymer Co 3 (hexaaminobenzene) 2 nanosheets for highly efficient oxygen evolution
    journal, January 2020

    • Li, Chun; Shi, Lingling; Zhang, Lili
    • Journal of Materials Chemistry A, Vol. 8, Issue 1
    • DOI: 10.1039/c9ta10644h

    A Dual‐Ligand Porous Coordination Polymer Chemiresistor with Modulated Conductivity and Porosity
    journal, January 2020

    • Yao, Ming‐Shui; Zheng, Jia‐Jia; Wu, Ai‐Qian
    • Angewandte Chemie International Edition, Vol. 59, Issue 1
    • DOI: 10.1002/anie.201909096

    Secondary‐Component Incorporated Hollow MOFs and Derivatives for Catalytic and Energy‐Related Applications
    journal, July 2018

    Robust heterostructures of a bimetallic sodium–zinc metal–organic framework and reduced graphene oxide for high-performance supercapacitors
    journal, January 2019

    • Rajak, Richa; Saraf, Mohit; Mobin, Shaikh M.
    • Journal of Materials Chemistry A, Vol. 7, Issue 4
    • DOI: 10.1039/c8ta09528k

    Synergistic effects of engineered spinel hetero-metallic cobaltites on electrochemical pseudo-capacitive behaviors
    journal, January 2018

    • Lee, Young-Woo; Hong, John; An, Geon-Hyoung
    • Journal of Materials Chemistry A, Vol. 6, Issue 31
    • DOI: 10.1039/c8ta04616f

    Origin of the Chemiresistive Response of Ultrathin Films of Conductive Metal–Organic Frameworks
    journal, November 2018

    • Rubio‐Giménez, Víctor; Almora‐Barrios, Neyvis; Escorcia‐Ariza, Garin
    • Angewandte Chemie International Edition, Vol. 57, Issue 46
    • DOI: 10.1002/anie.201808242

    Electroactive Metalorganic Frameworks
    journal, October 2018

    • Medina, Dana D.; Mähringer, Andre; Bein, Thomas
    • Israel Journal of Chemistry, Vol. 58, Issue 9-10
    • DOI: 10.1002/ijch.201800110

    Catalytic Metal Nanoparticles Embedded in Conductive Metal–Organic Frameworks for Chemiresistors: Highly Active and Conductive Porous Materials
    journal, August 2019

    • Koo, Won‐Tae; Kim, Sang‐Joon; Jang, Ji‐Soo
    • Advanced Science, Vol. 6, Issue 21
    • DOI: 10.1002/advs.201900250

    Recent Development and Application of Conductive MOFs
    journal, August 2018

    Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density
    journal, July 2018

    Morphology-dependent third-order optical nonlinearity of a 2D Co-based metal–organic framework with a porphyrinic skeleton
    journal, January 2019

    • Niu, Ru-Jie; Zhou, Wen-Fa; Liu, Yan
    • Chemical Communications, Vol. 55, Issue 33
    • DOI: 10.1039/c9cc01363f

    Titelbild: A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity (Angew. Chem. 13/2020)
    journal, January 2020

    • Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan
    • Angewandte Chemie, Vol. 132, Issue 13
    • DOI: 10.1002/ange.202001277

    A Phthalocyanine-Based Layered Two-Dimensional Conjugated Metal-Organic Framework as a Highly Efficient Electrocatalyst for the Oxygen Reduction Reaction
    journal, July 2019

    • Zhong, Haixia; Ly, Khoa Hoang; Wang, Mingchao
    • Angewandte Chemie International Edition, Vol. 58, Issue 31
    • DOI: 10.1002/anie.201907002

    Strain Redistribution in Metal‐Sulfide‐Composite Anode for Enhancing Volumetric Lithium Storage
    journal, October 2018

    Graphene-like metal-organic frameworks: Morphology control, optimization of thin film electrical conductivity and fast sensing applications
    other, January 2018

    • Hoppe, Bastian; Hindricks, Karen D. J.; Warwas, Dawid P.
    • Cambridge : Royal Society of Chemistry
    • DOI: 10.15488/4168

    Conductive Co-based metal–organic framework nanowires: a competitive high-rate anode towards advanced Li-ion capacitors
    journal, January 2019

    • Sun, Jinfeng; Guo, Lingzhi; Sun, Xuan
    • Journal of Materials Chemistry A, Vol. 7, Issue 43
    • DOI: 10.1039/c9ta08788e

    Hydrogen storage mechanism and diffusion in metal–organic frameworks
    journal, January 2019

    • Koizumi, Kenichi; Nobusada, Katsuyuki; Boero, Mauro
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 15
    • DOI: 10.1039/c8cp07467d

    Synaptic Plasticity and Filtering Emulated in Metal–Organic Frameworks Nanosheets Based Transistors
    journal, November 2019

    • Ding, Guanglong; Yang, Baidong; Zhou, Kui
    • Advanced Electronic Materials, Vol. 6, Issue 1
    • DOI: 10.1002/aelm.201900978

    Porous Ultrathin NiSe Nanosheet Networks on Nickel Foam for High‐Performance Hybrid Supercapacitors
    journal, October 2019

    Engineering Bimetal Synergistic Electrocatalysts Based on Metal–Organic Frameworks for Efficient Oxygen Evolution
    journal, September 2019

    Interfacial Approach toward Benzene‐Bridged Polypyrrole Film–Based Micro‐Supercapacitors with Ultrahigh Volumetric Power Density
    journal, December 2019

    • Jiang, Kaiyue; Baburin, Igor A.; Han, Peng
    • Advanced Functional Materials, Vol. 30, Issue 7
    • DOI: 10.1002/adfm.201908243

    Assembling laminated films via the synchronous reduction of graphene oxide and formation of copper-based metal organic frameworks
    journal, January 2019

    • Li, Li; Chen, Ruyi; Gong, Yujiao
    • Journal of Materials Chemistry A, Vol. 7, Issue 1
    • DOI: 10.1039/c8ta09065c

    Shape‐Assisted 2D MOF/Graphene Derived Hybrids as Exceptional Lithium‐Ion Battery Electrodes
    journal, July 2019

    • Jayaramulu, Kolleboyina; Dubal, Deepak P.; Schneemann, Andreas
    • Advanced Functional Materials, Vol. 29, Issue 38
    • DOI: 10.1002/adfm.201902539

    Two-dimensional metal–organic frameworks and their derivatives for electrochemical energy storage and electrocatalysis
    journal, January 2020

    • Zhao, Kuangmin; Zhu, Weiwei; Liu, Suqin
    • Nanoscale Advances, Vol. 2, Issue 2
    • DOI: 10.1039/c9na00719a
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