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Title: 3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

Abstract

Abstract The performance of pseudocapacitive electrodes at fast charging rates are typically limited by the slow kinetics of Faradaic reactions and sluggish ion diffusion in the bulk structure. This is particularly problematic for thick electrodes and electrodes highly loaded with active materials. Here, a surface‐functionalized 3D‐printed graphene aerogel (SF‐3D GA) is presented that achieves not only a benchmark areal capacitance of 2195 mF cm −2 at a high current density of 100 mA cm −2 but also an ultrahigh intrinsic capacitance of 309.1 µF cm −2 even at a high mass loading of 12.8 mg cm −2 . Importantly, the kinetic analysis reveals that the capacitance of SF‐3D GA electrode is primarily (93.3%) contributed from fast kinetic processes. This is because the 3D‐printed electrode has an open structure that ensures excellent coverage of functional groups on carbon surface and facilitates the ion accessibility of these surface functional groups even at high current densities and large mass loading/electrode thickness. An asymmetric device assembled with SF‐3D GA as anode and 3D‐printed GA decorated with MnO 2 as cathode achieves a remarkable energy density of 0.65 mWh cm −2 at an ultrahigh power density of 164.5 mW cm −2 , outperforming carbon‐based supercapacitorsmore » operated at the same power density.« less

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [3];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [1]
  1. Department of Chemistry and Biochemistry University of California Santa Cruz CA 95064 USA
  2. Lawrence Livermore National Laboratory 7000 East Avenue Livermore CA 94550 USA
  3. MOE of the Key Laboratory of Bioinorganic and Synthetic Chemistry The Key Lab of Low‐Carbon Chemistry &, Energy Conservation of Guangdong Province School of Chemistry Sun Yat‐Sen University Guangzhou 510275 P. R. China
  4. Department of Chemistry and Biochemistry University of California Santa Cruz CA 95064 USA, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1592185
Alternate Identifier(s):
OSTI ID: 1592186; OSTI ID: 1873250
Report Number(s):
LLNL-JRNL-801202; 16-ERD-051; 20-ERD-019
Journal ID: ISSN 0935-9648; 1906652
Grant/Contract Number:  
DE‐AC52‐07NA27344; AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials Journal Volume: 32 Journal Issue: 8; Journal ID: ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English
Subject:
42 ENGINEERING; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 3D printing; graphene aerogels; surface functionalization; intrinsic capacitance; asymmetric supercapacitors

Citation Formats

Yao, Bin, Chandrasekaran, Swetha, Zhang, Haozhe, Ma, Annie, Kang, Junzhe, Zhang, Lei, Lu, Xihong, Qian, Fang, Zhu, Cheng, Duoss, Eric B., Spadaccini, Christopher M., Worsley, Marcus A., and Li, Yat. 3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels. Germany: N. p., 2020. Web. doi:10.1002/adma.201906652.
Yao, Bin, Chandrasekaran, Swetha, Zhang, Haozhe, Ma, Annie, Kang, Junzhe, Zhang, Lei, Lu, Xihong, Qian, Fang, Zhu, Cheng, Duoss, Eric B., Spadaccini, Christopher M., Worsley, Marcus A., & Li, Yat. 3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels. Germany. https://doi.org/10.1002/adma.201906652
Yao, Bin, Chandrasekaran, Swetha, Zhang, Haozhe, Ma, Annie, Kang, Junzhe, Zhang, Lei, Lu, Xihong, Qian, Fang, Zhu, Cheng, Duoss, Eric B., Spadaccini, Christopher M., Worsley, Marcus A., and Li, Yat. Fri . "3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels". Germany. https://doi.org/10.1002/adma.201906652.
@article{osti_1592185,
title = {3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels},
author = {Yao, Bin and Chandrasekaran, Swetha and Zhang, Haozhe and Ma, Annie and Kang, Junzhe and Zhang, Lei and Lu, Xihong and Qian, Fang and Zhu, Cheng and Duoss, Eric B. and Spadaccini, Christopher M. and Worsley, Marcus A. and Li, Yat},
abstractNote = {Abstract The performance of pseudocapacitive electrodes at fast charging rates are typically limited by the slow kinetics of Faradaic reactions and sluggish ion diffusion in the bulk structure. This is particularly problematic for thick electrodes and electrodes highly loaded with active materials. Here, a surface‐functionalized 3D‐printed graphene aerogel (SF‐3D GA) is presented that achieves not only a benchmark areal capacitance of 2195 mF cm −2 at a high current density of 100 mA cm −2 but also an ultrahigh intrinsic capacitance of 309.1 µF cm −2 even at a high mass loading of 12.8 mg cm −2 . Importantly, the kinetic analysis reveals that the capacitance of SF‐3D GA electrode is primarily (93.3%) contributed from fast kinetic processes. This is because the 3D‐printed electrode has an open structure that ensures excellent coverage of functional groups on carbon surface and facilitates the ion accessibility of these surface functional groups even at high current densities and large mass loading/electrode thickness. An asymmetric device assembled with SF‐3D GA as anode and 3D‐printed GA decorated with MnO 2 as cathode achieves a remarkable energy density of 0.65 mWh cm −2 at an ultrahigh power density of 164.5 mW cm −2 , outperforming carbon‐based supercapacitors operated at the same power density.},
doi = {10.1002/adma.201906652},
journal = {Advanced Materials},
number = 8,
volume = 32,
place = {Germany},
year = {Fri Jan 17 00:00:00 EST 2020},
month = {Fri Jan 17 00:00:00 EST 2020}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1002/adma.201906652

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