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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]
  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 Lab., Menlo Park, CA (United States); Argonne National Lab. (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.
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
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.
@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 = {2018},
month = {1}
}

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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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  • Advanced Science, Vol. 6, Issue 21
  • DOI: 10.1002/advs.201900250

Conductive Metal–Organic Frameworks Selectively Grown on Laser‐Scribed Graphene for Electrochemical Microsupercapacitors
journal, April 2019

  • Wu, Hao; Zhang, Wenli; Kandambeth, Sharath
  • Advanced Energy Materials, Vol. 9, Issue 21
  • DOI: 10.1002/aenm.201900482

Multielectron-Transfer-based Rechargeable Energy Storage of Two-Dimensional Coordination Frameworks with Non-Innocent Ligands
journal, May 2018

  • Wada, Keisuke; Sakaushi, Ken; Sasaki, Sono
  • Angewandte Chemie, Vol. 130, Issue 29
  • DOI: 10.1002/ange.201802521

A One‐Dimensional π–d Conjugated Coordination Polymer for Sodium Storage with Catalytic Activity in Negishi Coupling
journal, September 2019


2D Semiconducting Metal–Organic Framework Thin Films for Organic Spin Valves
journal, November 2019


Conjugated Copper–Catecholate Framework Electrodes for Efficient Energy Storage
journal, December 2019


Conjugated Copper–Catecholate Framework Electrodes for Efficient Energy Storage
journal, December 2019

  • Liu, Jingjuan; Zhou, Yi; Xie, Zhen
  • Angewandte Chemie International Edition, Vol. 59, Issue 3
  • DOI: 10.1002/anie.201912642

A Redox‐Active 2D Metal–Organic Framework for Efficient Lithium Storage with Extraordinary High Capacity
journal, March 2020

  • Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan
  • Angewandte Chemie International Edition, Vol. 59, Issue 13
  • DOI: 10.1002/anie.201914395

Metal−Organic Frameworks for High‐Energy Lithium Batteries with Enhanced Safety: Recent Progress and Future Perspectives
journal, April 2019

  • Zhang, Xiahui; Dong, Panpan; Song, Min‐Kyu
  • Batteries & Supercaps, Vol. 2, Issue 7
  • DOI: 10.1002/batt.201900012

Recent Development and Application of Conductive MOFs
journal, August 2018


MOFs and COFs for Batteries and Supercapacitors
journal, October 2019


Hierarchical 3D electrodes for electrochemical energy storage
journal, December 2018


Reversible lithium storage in a porphyrin-based MOF (PCN-600) with exceptionally high capacity and stability
journal, January 2018

  • Sun, Lin; Xie, Jie; Chen, Zhidong
  • Dalton Transactions, Vol. 47, Issue 30
  • DOI: 10.1039/c8dt02161a

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

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

Redox-active metal–organic frameworks for energy conversion and storage
journal, January 2019

  • Calbo, Joaquín; Golomb, Matthias J.; Walsh, Aron
  • Journal of Materials Chemistry A, Vol. 7, Issue 28
  • DOI: 10.1039/c9ta04680a

2D molecular crystal lattices: advances in their synthesis, characterization, and application
journal, January 2019

  • Solomos, Marina A.; Claire, F. James; Kempa, Thomas J.
  • Journal of Materials Chemistry A, Vol. 7, Issue 41
  • DOI: 10.1039/c9ta06534b

Dense organic molecules/graphene network anodes with superior volumetric and areal performance for asymmetric supercapacitors
journal, January 2020

  • Zhang, Lina; Han, Daliang; Tao, Ying
  • Journal of Materials Chemistry A, Vol. 8, Issue 1
  • DOI: 10.1039/c9ta09941g

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

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

An Olefin‐Linked Covalent Organic Framework as a Flexible Thin‐Film Electrode for a High‐Performance Micro‐Supercapacitor
journal, August 2019

  • Xu, Junsong; He, Yafei; Bi, Shuai
  • Angewandte Chemie International Edition, Vol. 58, Issue 35
  • DOI: 10.1002/anie.201905713

Freestanding Lamellar Porous Carbon Stacks for Low‐Temperature‐Foldable Supercapacitors
journal, July 2019


Construction of cobaltous oxide/nickel–iron oxide electrodes with great cycle stability and high energy density for advanced asymmetry supercapacitor
journal, November 2019

  • Zhao, Yan; Chen, Yuan; Liu, Qingqing
  • Journal of Materials Science: Materials in Electronics, Vol. 30, Issue 24
  • DOI: 10.1007/s10854-019-02495-3

Multivalent metal ion hybrid capacitors: a review with a focus on zinc-ion hybrid capacitors
journal, January 2019

  • Dong, Liubing; Yang, Wang; Yang, Wu
  • Journal of Materials Chemistry A, Vol. 7, Issue 23
  • DOI: 10.1039/c9ta02678a

A two-dimensional semiconducting covalent organic framework with nickel( ii ) coordination for high capacitive performance
journal, January 2019

  • Li, Tao; Zhang, Wen-Da; Liu, Yong
  • Journal of Materials Chemistry A, Vol. 7, Issue 34
  • DOI: 10.1039/c9ta07194f

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

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

Efficient and tunable one-dimensional charge transport in layered lanthanide metal–organic frameworks
journal, November 2019

  • Skorupskii, Grigorii; Trump, Benjamin A.; Kasel, Thomas W.
  • Nature Chemistry, Vol. 12, Issue 2
  • DOI: 10.1038/s41557-019-0372-0

Recent progress in two-dimensional polymers for energy storage and conversion: design, synthesis, and applications
journal, January 2018

  • Xiao, Peitao; Xu, Yuxi
  • Journal of Materials Chemistry A, Vol. 6, Issue 44
  • DOI: 10.1039/c8ta02820f

ZIF-8/ZIF-67-derived 3D amorphous carbon-encapsulated CoS/NCNTs supported on CoS-coated carbon nanofibers as an advanced potassium-ion battery anode
journal, January 2019

  • Miao, Wenfang; Zhang, Yu; Li, Haotian
  • Journal of Materials Chemistry A, Vol. 7, Issue 10
  • DOI: 10.1039/c8ta12457d

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

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

  • Jiang, Qiang; Xiong, Peixun; Liu, Jingjuan
  • Angewandte Chemie International Edition, Vol. 59, Issue 13
  • DOI: 10.1002/anie.202001277

A One‐Dimensional π–d Conjugated Coordination Polymer for Sodium Storage with Catalytic Activity in Negishi Coupling
journal, September 2019

  • Chen, Yuan; Tang, Mi; Wu, Yanchao
  • Angewandte Chemie International Edition, Vol. 58, Issue 41
  • DOI: 10.1002/anie.201908274

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.