Supercapacitors Based on Three-Dimensional Hierarchical Graphene Aerogels with Periodic Macropores

Zhu, Cheng; Liu, Tianyu; Qian, Fang; Han, T. Yong-Jin; Duoss, Eric B.; Kuntz, Joshua D.; Spadaccini, Christopher M.; Worsley, Marcus A.; Li, Yat

doi:10.1021/acs.nanolett.5b04965

Title: Supercapacitors Based on Three-Dimensional Hierarchical Graphene Aerogels with Periodic Macropores

Journal Article · Thu Jan 28 00:00:00 EST 2016 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.5b04965· OSTI ID:1809159

Zhu, Cheng ^[1]; Liu, Tianyu ^[2]; Qian, Fang ^[1]; Han, T. Yong-Jin ^[1]; Duoss, Eric B. ^[1]; Kuntz, Joshua D. ^[1]; Spadaccini, Christopher M. ^[1]; Worsley, Marcus A. ^[1]; Li, Yat ^[2]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of California, Santa Cruz, CA (United States)

Graphene is an atomically thin, two-dimensional (2D) carbon material that offers a unique combination of low density, exceptional mechanical properties, thermal stability, large surface area, and excellent electrical conductivity. Recent progress has resulted in macro-assemblies of graphene, such as bulk graphene aerogels for a variety of applications. However, these three-dimensional (3D) graphenes exhibit physicochemical property attenuation compared to their 2D building blocks because of one-fold composition and tortuous, stochastic porous networks. These limitations can be offset by developing a graphene composite material with an engineered porous architecture. In this work, we report the fabrication of 3D periodic graphene composite aerogel microlattices for supercapacitor applications, via a 3D printing technique known as direct-ink writing. The key factor in developing these novel aerogels is creating an extrudable graphene oxide-based composite ink and modifying the 3D printing method to accommodate aerogel processing. The 3D-printed graphene composite aerogel (3D-GCA) electrodes are lightweight, highly conductive, and exhibit excellent electrochemical properties. In particular, the supercapacitors using these 3D-GCA electrodes with thicknesses on the order of millimeters display exceptional capacitive retention (ca. 90% from 0.5 to 10 A·g^–1) and power densities (>4 kW·kg^–1) that equal or exceed those of reported devices made with electrodes 10–100 times thinner. This work provides an example of how 3D-printed materials, such as graphene aerogels, can significantly expand the design space for fabricating high-performance and fully integrable energy storage devices optimized for a broad range of applications.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1809159

Report Number(s):: LLNL-JRNL-720298; 860189

Journal Information:: Nano Letters, Vol. 16, Issue 6; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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3D Heteroatom‐Doped Carbon Nanomaterials as Multifunctional Metal‐Free Catalysts for Integrated Energy Devices Paul, Rajib; Du, Feng; Dai, Liming Advanced Materials, Vol. 31, Issue 13 https://doi.org/10.1002/adma.201805598	journal	January 2019
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3D Printing of Ultralight Biomimetic Hierarchical Graphene Materials with Exceptional Stiffness and Resilience Peng, Meiwen; Wen, Zhen; Xie, Lingjie Advanced Materials, Vol. 31, Issue 35 https://doi.org/10.1002/adma.201902930	journal	July 2019
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A 3D‐Printed Electrochemical Water Splitting Cell Lee, Chong‐Yong; Taylor, Adam C.; Beirne, Stephen Advanced Materials Technologies, Vol. 4, Issue 10 https://doi.org/10.1002/admt.201900433	journal	August 2019
Paper-Based Electrodes for Flexible Energy Storage Devices Yao, Bin; Zhang, Jing; Kou, Tianyi Advanced Science, Vol. 4, Issue 7 https://doi.org/10.1002/advs.201700107	journal	May 2017
Advanced Materials for Printed Wearable Electrochemical Devices: A Review Kim, Jayoung; Kumar, Rajan; Bandodkar, Amay J. Advanced Electronic Materials, Vol. 3, Issue 1 https://doi.org/10.1002/aelm.201600260	journal	December 2016
Biomimetic and Radially Symmetric Graphene Aerogel for Flexible Electronics Gao, Libo; Fan, Rong; Zhou, Wenzhao Advanced Electronic Materials, Vol. 5, Issue 12 https://doi.org/10.1002/aelm.201900353	journal	August 2019
Nature-Inspired Electrochemical Energy-Storage Materials and Devices Wang, Hua; Yang, Yun; Guo, Lin Advanced Energy Materials, Vol. 7, Issue 5 https://doi.org/10.1002/aenm.201601709	journal	December 2016
Battery-like Supercapacitors from Vertically Aligned Carbon Nanofiber Coated Diamond: Design and Demonstrator Yu, Siyu; Yang, Nianjun; Vogel, Michael Advanced Energy Materials, Vol. 8, Issue 12 https://doi.org/10.1002/aenm.201702947	journal	January 2018
3D Printing Quasi-Solid-State Asymmetric Micro-Supercapacitors with Ultrahigh Areal Energy Density Shen, Kai; Ding, Junwei; Yang, Shubin Advanced Energy Materials, Vol. 8, Issue 20 https://doi.org/10.1002/aenm.201800408	journal	April 2018
Engineering of Mesoscale Pores in Balancing Mass Loading and Rate Capability of Hematite Films for Electrochemical Capacitors Song, Yu; Liu, Tianyu; Li, Mingyang Advanced Energy Materials, Vol. 8, Issue 26 https://doi.org/10.1002/aenm.201801784	journal	August 2018
3D Printing of Tunable Energy Storage Devices with Both High Areal and Volumetric Energy Densities Gao, Tingting; Zhou, Zhan; Yu, Jianyong Advanced Energy Materials, Vol. 9, Issue 8 https://doi.org/10.1002/aenm.201802578	journal	December 2018
3D Printing of Electrochemical Energy Storage Devices: A Review of Printing Techniques and Electrode/Electrolyte Architectures Cheng, Meng; Deivanayagam, Ramasubramonian; Shahbazian‐Yassar, Reza Batteries & Supercaps, Vol. 3, Issue 2 https://doi.org/10.1002/batt.201900130	journal	November 2019
Hybrid Iron Oxide on Three-Dimensional Exfoliated Graphite Electrode with Ultrahigh Capacitance for Energy Storage Applications Sun, Zhen; Cai, Xiang; Feng, Dong-Yang ChemElectroChem, Vol. 5, Issue 11 https://doi.org/10.1002/celc.201800143	journal	April 2018
Functional Inks for Printable Energy Storage Applications based on 2 D Materials Wang, Libin; Chen, Shi; Shu, Ting ChemSusChem, Vol. 13, Issue 6 https://doi.org/10.1002/cssc.201902019	journal	March 2020
Nitrogen‐doped self‐shrinking porous 3D graphene capacitor deionization electrode Qian, Ming; Duan, Mengna; Gong, Zuode International Journal of Energy Research https://doi.org/10.1002/er.4741	journal	July 2019
Multifaceted polymeric materials in three-dimensional processing (3DP) technologies: Current progress and prospects Oderinde, Olayinka; Liu, Shunli; Li, Kewen Polymers for Advanced Technologies, Vol. 29, Issue 6 https://doi.org/10.1002/pat.4281	journal	March 2018
3D printing of conjugated polymers Jordan, Robert S.; Wang, Yue Journal of Polymer Science Part B: Polymer Physics, Vol. 57, Issue 23 https://doi.org/10.1002/polb.24893	journal	August 2019
Recent Advances in 3D Graphene Architectures and Their Composites for Energy Storage Applications Wang, Zhijie; Gao, Hong; Zhang, Qing Small https://doi.org/10.1002/smll.201803858	journal	December 2018
Cellulose-Nanofiber-Enabled 3D Printing of a Carbon-Nanotube Microfiber Network Li, Yuanyuan; Zhu, Hongli; Wang, Yibo Small Methods, Vol. 1, Issue 10 https://doi.org/10.1002/smtd.201700222	journal	September 2017
Recent Advances in Design of Flexible Electrodes for Miniaturized Supercapacitors Yu, Chenyang; An, Jianing; Chen, Qiang Small Methods, Vol. 4, Issue 6 https://doi.org/10.1002/smtd.201900824	journal	February 2020
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Mechanical and microwave absorption properties of 3D-printed Li0.44Zn0.2Fe2.36O4/polylactic acid composites using fused deposition modeling Qian, Yi; Yao, Zhengjun; Lin, Haiyan Journal of Materials Science: Materials in Electronics, Vol. 29, Issue 22 https://doi.org/10.1007/s10854-018-0056-3	journal	September 2018
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3D Printed Graphene Based Energy Storage Devices Foster, Christopher W.; Down, Michael P.; Zhang, Yan Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/srep42233	journal	March 2017
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A general gelation strategy for 1D nanowires: dynamically stable functional gels for 3D printing flexible electronics Liu, Shuiren; Shi, Xinlei; Li, Xiran Nanoscale, Vol. 10, Issue 43 https://doi.org/10.1039/c8nr06369a	journal	January 2018
Electrochemical synthesis of NiCo layered double hydroxide nanosheets decorated on moderately oxidized graphene films for energy storage Jia, Dedong; Jiang, Degang; Zheng, Yiwei Nanoscale, Vol. 11, Issue 6 https://doi.org/10.1039/c8nr08869a	journal	January 2019
Synthesis of C/Co ₃ O ₄ composite mesoporous hollow sphere sandwich graphene films for high-performance supercapacitors Sun, Lin; Yan, Ming; Xiao, Lisong Inorganic Chemistry Frontiers, Vol. 5, Issue 10 https://doi.org/10.1039/c8qi00559a	journal	January 2018
Heteroatom-doped carbon materials and their composites as electrocatalysts for CO ₂ reduction Cui, Huijuan; Guo, Yibo; Guo, Limin Journal of Materials Chemistry A, Vol. 6, Issue 39 https://doi.org/10.1039/c8ta07430e	journal	January 2018
Continuously 3D printed quantum dot-based electrodes for lithium storage with ultrahigh capacities Zhang, Chao; Shen, Kai; Li, Bin Journal of Materials Chemistry A, Vol. 6, Issue 41 https://doi.org/10.1039/c8ta08559e	journal	January 2018
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Fe ₃ O ₄ hard templating to assemble highly wrinkled graphene sheets into hierarchical porous film for compact capacitive energy storage Fang, Hua; Meng, Fanteng; Yan, Ji RSC Advances, Vol. 9, Issue 35 https://doi.org/10.1039/c9ra02132a	journal	January 2019
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MOF-derived conductive carbon nitrides for separator-modified Li–S batteries and flexible supercapacitors Cai, Jingsheng; Song, Yingze; Chen, Xiang Journal of Materials Chemistry A, Vol. 8, Issue 4 https://doi.org/10.1039/c9ta11958b	journal	January 2020
Electrochemical in situ construction of vanadium oxide heterostructures with boosted pseudocapacitive charge storage Dong, Ran; Song, Yu; Yang, Duo Journal of Materials Chemistry A, Vol. 8, Issue 3 https://doi.org/10.1039/c9ta12097a	journal	January 2020
Block copolymers for supercapacitors, dielectric capacitors and batteries Liu, Tianyu; Liu, Guoliang Journal of Physics: Condensed Matter, Vol. 31, Issue 23 https://doi.org/10.1088/1361-648X/ab0d77	journal	March 2019
3D printed nanomaterial-based electronic, biomedical, and bioelectronic devices Hales, Samuel; Tokita, Eric; Neupane, Rajan Nanotechnology, Vol. 31, Issue 17 https://doi.org/10.1088/1361-6528/ab5f29	journal	February 2020
Carbon-based supercapacitors for efficient energy storage Chen, Xuli; Paul, Rajib; Dai, Liming National Science Review, Vol. 4, Issue 3 https://doi.org/10.1093/nsr/nwx009	journal	March 2017
Digested sludge-derived three-dimensional hierarchical porous carbon for high-performance supercapacitor electrode Zhang, Jia-Jia; Fan, Hao-Xiang; Dai, Xiao-Hu Royal Society Open Science, Vol. 5, Issue 4 https://doi.org/10.1098/rsos.172456	journal	April 2018
Toward digitally controlled catalyst architectures: Hierarchical nanoporous gold via 3D printing Zhu, Cheng; Qi, Zhen; Beck, Victor A. Science Advances, Vol. 4, Issue 8 https://doi.org/10.1126/sciadv.aas9459	journal	August 2018
Carbon aerogel evolution: Allotrope, graphene-inspired, and 3D-printed aerogels Chandrasekaran, Swetha; Campbell, Patrick G.; Baumann, Theodore F. Journal of Materials Research, Vol. 32, Issue 22 https://doi.org/10.1557/jmr.2017.411	journal	October 2017
Nanostructured resorcinol-formaldehyde ink for 3D direct writing Ge, Yingting; Zhang, Ting; Zhou, Bin Journal of Materials Research, Vol. 33, Issue 14 https://doi.org/10.1557/jmr.2018.104	journal	May 2018
Functional inks and printing of two-dimensional materials. Hu, Guohua; Kang, Joohoon; Ng, Leonard WT Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.24846	text	January 2018
Activated Carbon in the Third Dimension—3D Printing of a Tuned Porous Carbon Steldinger, Hendryk; Esposito, Alessandro; Brunnengräber, Kai Wiley VCH https://doi.org/10.25534/tuprints-00011603	text	January 2019
Synthesis of Three-Dimensional Graphene-Based Hybrid Materials for Water Purification: A Review Wang, Yan; Guo, Lei; Qi, Pengfei Nanomaterials, Vol. 9, Issue 8 https://doi.org/10.3390/nano9081123	journal	August 2019
Anchoring Fe ₃ O ₄ nanoparticles in a reduced graphene oxide aerogel matrix via polydopamine coating Scheibe, Błażej; Mrówczyński, Radosław; Michalak, Natalia Beilstein Journal of Nanotechnology, Vol. 9 https://doi.org/10.3762/bjnano.9.55	journal	January 2018
Activated Carbon in the Third Dimension—3D Printing of a Tuned Porous Carbon Steldinger, Hendryk; Esposito, Alessandro; Brunnengräber, Kai Advanced Science, Vol. 6, Issue 19 https://doi.org/10.1002/advs.201901340	journal	August 2019
Double-Crosslinked GO Interlayer Framework as a Pervaporation Hybrid Membrane with High Performance Zhang, Xin; Zhang, Ming-Xiao; Ding, Hao ACS Omega, Vol. 4, Issue 12 https://doi.org/10.1021/acsomega.9b01833	journal	September 2019
Fast ion transport through ultrathin shells of metal sulfide hollow nanocolloids used for high-performance energy storage Chen, Zhenhua; Zhao, Mengen; Lv, Xinyan Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-017-18504-6	journal	January 2018
Ultralight Graphene/Carbon Nanotubes Aerogels with Compressibility and Oil Absorption Properties Zhao, Da; Yu, Li; Liu, Dongxu Materials, Vol. 11, Issue 4 https://doi.org/10.3390/ma11040641	journal	April 2018

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