Combustion-Assisted Photonic Annealing of Printable Graphene Inks

Aug 18, 2017 - ‡Department of Materials Science and Engineering and ⊥Department of Chemistry, Department of Electrical Engineering and Computer Sc...
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Combustion-Assisted Photonic Annealing of Printable Graphene Inks via Exothermic Binders Ethan B. Secor, Theodore Z. Gao, Manuel H Dos Santos, Shay G Wallace, Karl W Putz, and Mark C Hersam ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.7b07189 • Publication Date (Web): 18 Aug 2017 Downloaded from http://pubs.acs.org on August 19, 2017

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Combustion-Assisted Photonic Annealing of Printable Graphene Inks via Exothermic Binders Ethan B. Secor†,#, Theodore Z. Gao†,#, , Manuel H. Dos Santos†, Shay G. Wallace†, Karl W. Putz†, and Mark C. Hersam†, §, * † Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208, United States § Department of Chemistry, Department of Electrical Engineering and Computer Science, Northwestern University, Evanston, IL 60208, United States Present address: Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305-4034, United States # These authors contributed equally to this work. * Corresponding Author: [email protected]

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Abstract

High-throughput and low-temperature processing of high performance nanomaterial inks is an important technical challenge for large-area, flexible printed electronics. In this report, we demonstrate nitrocellulose as an exothermic binder for photonic annealing of conductive graphene inks, leveraging the rapid decomposition kinetics and built-in energy of nitrocellulose to enable versatile process integration. This strategy results in superlative electrical properties that are comparable to extended thermal annealing at 350 °C, using a pulsed light process that is compatible with thermally sensitive substrates. The resulting porous microstructure and broad liquid-phase patterning compatibility are exploited for printed graphene microsupercapacitors on paper-based substrates.

Keywords: carbon nanomaterials; conductive inks; energetic materials; intense pulsed light annealing; printed electronics

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Additive manufacturing of electronically functional materials offers compelling benefits for printed electronics, with applications in energy technologies, biomedical diagnostics, and the Internet of Things.1,2 With advanced direct-write capabilities, complicated digital designs can be fabricated with low cost, minimal waste, and high resolution.3,4 A key obstacle to the widespread adoption of this technology is the development of functional liquid inks with compatible printing and process integration. Among conductive inks, graphene has attracted considerable interest as a result of its high electrical and thermal conductivity, mechanical flexibility, and chemical and environmental stability.5,6 Pristine graphene can be exfoliated from flake graphite using scalable, liquid-phase processing methods, such as shear mixing, coupled with engineered solvent and dispersant systems.7,8 The use of polymer dispersants is particularly promising for downstream integration in printing processes, since the polymer offers high colloidal stability and an adjustable parameter to tailor fluid properties for specific printing methods.9 In this way, versatile and high performance graphene inks have been designed for a range of liquid-phase printing methods.10–12 Despite the aforementioned advantages of polymer-stabilized graphene inks, the resulting printed structures require annealing to decompose the dispersant, which can present process integration limitations. In particular, traditional thermal processing limits process speed and compatibility with temperature-sensitive materials. As a result, a pulsed photonic annealing method (i.e., intense pulsed light annealing), has been demonstrated for rapid processing on thermally sensitive substrates, with straightforward integration in roll-to-roll processing.13–18 This method employs a broadband pulsed light source, typically a xenon arc lamp, to produce high-intensity (~1-5 kW/cm2) light pulses with durations on the order of milliseconds. Preferential optical absorption within the active film leads to rapid local heating that limits

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thermal damage to passive components such as the underlying substrate. While the initial results on photonic annealing of printable graphene inks have been promising, optimal utilization of this technique requires complementary ink properties tailored to the annealing method. Toward that end, here we demonstrate a graphene ink designed for pulsed light annealing based on the polymer binder nitrocellulose, which exhibits rapid and exothermic decomposition. This approach enables highly conductive and porous graphene patterns with broad process compatibility and superlative performance metrics in addition to establishing a compelling ink design strategy for broader application in photonic annealing. The design of graphene inks for photonic annealing draws inspiration from literature precedent in the fields of thin film metal oxide electronics and ceramic synthesis. In this context, combustion processing of metal oxide thin-film transistors has been demonstrated by careful selection of exothermic precursors that lower the energy barrier for annealing and densification, ultimately yielding desirable performance with reduced processing temperatures.19 In ceramic materials, the technique of self-propagating high-temperature synthesis (SHS) similarly uses a locally-initiated combustion wave to achieve thermal processing in a rapid and efficient manner.20 Since the decomposition of reactive precursors leads to gas evolution, this approach is particularly effective for producing porous, high surface-area morphologies.21 In order to use photonic annealing to initiate combustion reactions in graphene inks, a reactive binder is required that undergoes rapid, exothermic decomposition. A promising candidate is nitrocellulose (NC), which has recently been shown to effectively disperse graphene, providing stable inks with graphene concentrations up to 10% w/v.22 In addition, the oxidizing nitrate groups of NC afford high chemical reactivity that favors exothermic decomposition with rapid kinetics that are consistent with photonic annealing (Figure 1a).23,24 Due to its rapid and exothermic

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decomposition, NC acts as an intrinsic energy source to fuel a propagating reaction, with positive implications for process generality. Moreover, the evolution of volatile gaseous species upon NC decomposition leads to a highly porous microstructure, offering advantages for applications such as energy storage, catalysis, and sensing.25,26

Figure 1. Process overview and proof of concept. (a) Chemical structure of nitrocellulose (left) and graphene (right). (b) Differential scanning calorimetry of graphene/nitrocellulose showing the large exothermic reaction of nitrocellulose at ~200 °C. (c) Schematic illustration of photonic annealing, which initiates a nitrocellulose propagating reaction. Cross-sectional scanning electron microscopy reveals the resulting porous graphene microstructure even on a thermally conductive silicon substrate.

The composite graphene/NC powder is produced by high shear mixing, centrifugation, and flocculation steps as previously reported (detailed experimental methods are provided in the

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Supporting Information).22 This procedure yields a powder containing ~35 wt. % graphene flakes with a typical thickness of ~2 nm and lateral size of ~300 nm (Supporting Information, Figure S1a). During photonic annealing, the strongly absorbing graphene film will undergo rapid photothermal heating primarily near the surface, and this heat will dissipate through the bulk of the film. For the suggested propagating reaction to occur, the energy released upon NC decomposition must be sufficiently greater than the energy required to initiate the decomposition reaction. Differential scanning calorimetry (DSC) results shown in Figure 1b indicate that NC decomposes exothermically at ~200 °C, releasing ~3x more energy than the amount required to heat the material to the decomposition temperature, which suggests that the NC combustion will likely propagate once locally initiated. In contrast, a control sample of graphene/ethyl cellulose (EC), a common dispersant for graphene inks,9 exhibits endothermic decomposition characteristics (Figure S1b). The differences in reaction kinetics and thermodynamics between NC and EC are further demonstrated by a photonic annealing test on a silicon substrate. Importantly, photonic annealing is traditionally limited to substrates that act as poor heat sinks, such as paper and plastic. Substrates with higher thermal mass and thermal conductivity, such as silicon, extract heat out of the active film rapidly to quench the process, limiting its applicability.15,13 However, the high exothermicity of NC combustion enables photonic annealing on silicon, while the rapid release of volatile decomposition products leads to a porous microstructure, as shown in the cross-sectional scanning electron microscopy (SEM) image in Figure 1c. Although the bottom portion of the film (90% capacitance retention following 1000 cycles (Figure 4f). In summary, we have demonstrated rapid photonic annealing of graphene/NC films, in which the exothermic NC binder acts as a built-in energy source to assist the annealing reaction. Chemical and electrical characterization reveals effective annealing with a single millisecond light pulse, resulting in properties comparable to extended thermal annealing at 350 °C. Moreover, the rapid volatilization of the NC binder leads to a porous microstructure, providing enhanced surface area for applications such as energy storage, sensing, and catalysis. The favorable process compatibility of this method is leveraged in combination with the versatile liquid-phase processing platform for graphene inks, enabling direct ink writing of printed solid-

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state graphene microsupercapacitors on flexible substrates such as glassine paper. While particularly useful for graphene inks, the attributes of NC as a synergistic binder for photonic annealing can likely be generalized to other material systems of interest to additive manufacturing. ASSOCIATED CONTENT Supporting Information. Detailed experimental procedure; characterization of control graphene/EC samples with DSC, SEM, and electrical measurements; and additional thermal, chemical, rheological, and electrochemical characterization can be found in the Supporting Information. This material is available free of charge via the Internet at http://pubs.acs.org.

AUTHOR INFORMATION Corresponding Author *Mark C. Hersam: [email protected] ORCID Mark C. Hersam: 0000-0003-4120-1426 Ethan B. Secor: 0000-0003-2324-1686 Theodore Z. Gao: 0000-0002-5217-5027 Shay G. Wallace: 0000-0002-7535-6138

Present Address

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Department of Materials Science and Engineering, Stanford University, Stanford, CA 943054034, United States Author Contributions # E.B.S. and T.Z.G. contributed equally to this work. Notes The authors declare no competing financial interests.

ACKNOWLEDGEMENT E.B. Secor and T.Z. Gao contributed equally to this work. This work was supported by the Air Force Research Laboratory under agreement number FA8650-15-2-5518. EBS was further supported by the Department of Defense (DoD) through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program, the Ryan Fellowship administered through the Northwestern University International Institute for Nanotechnology, and the Cabell Terminal Year Fellowship. This work made use of the EPIC and Keck-II facilities within the Northwestern University NUANCE Center, which has received support from the NSF Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (ECCS-1542205); the NSF MRSEC program (DMR-1121262); the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois. TGA and DSC were performed in the Materials Characterization and Imaging facility at Northwestern University, which receives support from the NSF MRSEC (DMR-1121262). The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and

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conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of the sponsors.

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References (1)

Arias, A. C.; MacKenzie, J. D.; McCulloch, I.; Rivnay, J.; Salleo, A. Materials and

Applications for Large Area Electronics: Solution-Based Approaches. Chem. Rev. 2010, 110, 3– 24. (2)

Nathan, A.; Ahnood, A.; Cole, M. T.; Suzuki, Y.; Hiralal, P.; Bonaccorso, F.; Hasan, T.;

Garcia-Gancedo, L.; Dyadyusha, A.; Haque, S.; Andrew, P.; Hofmann, S.; Moultrie, J.; Chu, D.; Flewitt, A. J.; Ferrari, A. C.; Kelly, M. J.; Robertson, J.; Amaratunga, G. A. J.; Milne, W. I. Flexible Electronics: The Next Ubiquitous Platform. Proc. IEEE 2012, 100, 1486–1517. (3)

Sarobol, P.; Cook, A.; Clem, P. G.; Keicher, D.; Hirschfeld, D.; Hall, A. C.; Bell, N. S.

Additive Manufacturing of Hybrid Circuits. Annu. Rev. Mater. Res. 2016, 46, 41–62. (4)

Lupo, D.; Clemens, W.; Breitung, S.; Hecker, K. Applications of Organic and Printed

Electronics. In Applications of Organic and Printed Electronics: A Technology-Enabled Revolution; Cantatore, E., Ed.; Springer US: Boston, MA, 2013; pp 1–26. (5)

Zhu, J.; Hersam, M. C. Assembly and Electronic Applications of Colloidal

Nanomaterials. Adv. Mater. 2017, 29, 1603895. (6)

Bonaccorso, F.; Bartolotta, A.; Coleman, J. N.; Backes, C. 2D-Crystal-Based Functional

Inks. Adv. Mater. 2016, 28, 6136–6166. (7)

Ciesielski, A.; Samorì, P. Graphene via Sonication Assisted Liquid-Phase Exfoliation.

Chem. Soc. Rev. 2014, 43, 381–398. (8)

Paton, K. R.; Varrla, E.; Backes, C.; Smith, R. J.; Khan, U.; O’Neill, A.; Boland, C.;

Lotya, M.; Istrate, O. M.; King, P.; Higgins, T.; Barwich, S.; May, P.; Puczkarski, P.; Ahmed, I.;

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1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 18 of 22

Moebius, M.; Petterson, H.; Long, E.; Coelho, J.; O'Brien, S. E.; McGuire, E. K.; Sanchez, B. M.; Duesberg, G. S.; McEvoy, N.; Pennycook, T. J; Downing, C.; Crossley, A.; Nicolosi, V.; Coleman, J. N.. Scalable Production of Large Quantities of Defect-Free Few-Layer Graphene by Shear Exfoliation in Liquids. Nat. Mater. 2014, 13, 624-630. (9)

Secor, E. B.; Hersam, M. C. Emerging Carbon and Post-Carbon Nanomaterial Inks for

Printed Electronics. J. Phys. Chem. Lett. 2015, 6, 620–626. (10)

Secor, E. B.; Prabhumirashi, P. L.; Puntambekar, K.; Geier, M. L.; Hersam, M. C. Inkjet

Printing of High Conductivity, Flexible Graphene Patterns. J. Phys. Chem. Lett. 2013, 4, 1347– 1351. (11)

Secor, E. B.; Lim, S.; Zhang, H.; Frisbie, C. D.; Francis, L. F.; Hersam, M. C. Gravure

Printing of Graphene for Large-Area Flexible Electronics. Adv. Mater. 2014, 26, 4533–4538. (12)

Hyun, W. J.; Secor, E. B.; Hersam, M. C.; Frisbie, C. D.; Francis, L. F. High-Resolution

Patterning of Graphene by Screen Printing with a Silicon Stencil for Highly Flexible Printed Electronics. Adv. Mater. 2015, 27, 109–115. (13)

Schroder, K. A. Mechanisms of Photonic CuringTM: Processing High Temperature Films

on Low Temperature Substrates. Technical Proceedings of the 2011 NSTI Nanotechnology Conference and Trade Show 2011, 2, 220–223. (14)

Schroder, K. A.; McCool, S. C.; Furlan, W. F. Broadcast Photonic Curing of Metallic

Nanoparticle Films. Technical Proceedings of the 2006 NSTI Nanotechnology Conference and Trade Show 2006, 3, 198–201. (15)

Wunscher, S.; Abbel, R.; Perelaer, J.; Schubert, U. S. Progress of Alternative Sintering

ACS Paragon Plus Environment

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Page 19 of 22

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Applied Materials & Interfaces

Approaches of Inkjet-Printed Metal Inks and Their Application for Manufacturing of Flexible Electronic Devices. J. Mater. Chem. C 2014, 2, 10232–10261. (16)

Secor, E. B.; Ahn, B. Y.; Gao, T. Z.; Lewis, J. A.; Hersam, M. C. Rapid and Versatile

Photonic Annealing of Graphene Inks for Flexible Printed Electronics. Adv. Mater. 2015, 27, 6683–6688. (17)

Arapov, K.; Bex, G.; Hendriks, R.; Rubingh, E.; Abbel, R.; de With, G.; Friedrich, H.

Conductivity Enhancement of Binder-Based Graphene Inks by Photonic Annealing and Subsequent Compression Rolling. Adv. Eng. Mater. 2016, 18, 1234–1239. (18)

Paglia, F.; Vak, D.; Van Embden, J.; Chesman, A. S. R.; Martucci, A.; Jasieniak, J. J.;

Della Gaspera, E. Photonic Sintering of Copper through the Controlled Reduction of Printed CuO Nanocrystals. ACS Appl. Mater. Interfaces 2015, 7, 25473–25478. (19)

Kim, M.-G.; Kanatzidis, M. G.; Facchetti, A.; Marks, T. J. Low-Temperature Fabrication

of High-Performance Metal Oxide Thin-Film Electronics via Combustion Processing. Nat. Mater. 2011, 10, 382–388. (20)

Merzhanov, A. G. History and Recent Developments in SHS. Ceram. Int. 1995, 21, 371–

379. (21)

Li, F.; Ran, J.; Jaroniec, M.; Qiao, S. Z. Solution Combustion Synthesis of Metal Oxide

Nanomaterials for Energy Storage and Conversion. Nanoscale 2015, 7, 17590–17610. (22)

Secor, E. B.; Gao, T. Z.; Islam, A. E.; Rao, R.; Wallace, S. G.; Zhu, J.; Putz, K. W.;

Maruyama, B.; Hersam, M. C. Enhanced Conductivity, Adhesion, and Environmental Stability of Printed Graphene Inks with Nitrocellulose. Chem. Mater. 2017, 29, 2332–2340.

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(23)

Page 20 of 22

Brill, T. B.; Gongwer, P. E. Thermal Decomposition of Energetic Materials 69. Analysis

of the Kinetics of Nitrocellulose at 50 °C-500 °C. Propellants, Explos. Pyrotech. 1997, 22, 38– 44. (24)

Taylor, J.; Hall, C. R. L. Determination of the Heat of Combustion of Nitroglycerin and

the Thermochemical Constants of Nitrocellulose. J. Phys. Chem. 1947, 51, 593–611. (25)

Zhang, X.; Ziemer, K. S.; Zhang, K.; Ramirez, D.; Li, L.; Wang, S.; Hope-Weeks, L. J.;

Weeks, B. L. Large-Area Preparation of High-Quality and Uniform Three-Dimensional Graphene Networks through Thermal Degradation of Graphene Oxide-Nitrocellulose Composites. ACS Appl. Mater. Interfaces 2015, 7, 1057–1064. (26)

Rao, C. N. R.; Gopalakrishnan, K.; Maitra, U. Comparative Study of Potential

Applications of Graphene, MoS2, and Other Two-Dimensional Materials in Energy Devices, Sensors, and Related Areas. ACS Appl. Mater. Interfaces 2015, 7, 7809–7832. (27)

Hyun, W. J.; Secor, E. B.; Rojas, G. A.; Hersam, M. C.; Francis, L. F.; Frisbie, C. D. All-

Printed, Foldable Organic Thin-Film Transistors on Glassine Paper. Adv. Mater. 2015, 27, 7058– 7064. (28)

Lin, Y.; Gritsenko, D.; Liu, Q.; Lu, X.; Xu, J. Recent Advancements in Functionalized

Paper-Based Electronics. ACS Appl. Mater. Interfaces 2016, 8, 20501–20515. (29)

Mahadeva, S. K.; Walus, K.; Stoeber, B. Paper as a Platform for Sensing Applications

and Other Devices: A Review. ACS Appl. Mater. Interfaces 2015, 7, 8345–8362. (30)

Lewis, J. A. Direct-Write Assembly of Ceramics from Colloidal Inks. Curr. Opin. Solid

State Mater. Sci. 2002, 6, 245–250.

ACS Paragon Plus Environment

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(31)

Li, L.; Secor, E. B.; Chen, K.; Zhu, J.; Liu, X.; Gao, T. Z.; Seo, J. T.; Zhao, Y.; Hersam,

M. C. High-Performance Solid-State Supercapacitors and Microsupercapacitors Derived from Printable Graphene Inks. Adv. Energy Mater. 2016, 6, 1600909. (32)

Li, J.; Ye, F.; Vaziri, S.; Muhammed, M.; Lemme, M. C.; Östling, M. Efficient Inkjet

Printing of Graphene. Adv. Mater. 2013, 25, 3985–3992. (33)

Li, J.; Mishukova, V.; Östling, M. All-Solid-State Micro-Supercapacitors Based on Inkjet

Printed Graphene Electrodes. Appl. Phys. Lett. 2016, 109, 123901.

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