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A Sequential Process of Graphene Exfoliation and Site-Selective Copper/Graphene Metallization Enabled by Multifunctional 1-Pyrenebutyric Acid Tetrabutylammonium Salt
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics. Northwest Univ, Coll Chem & Mat Sci, Minist Educ, Key Lab Synthet & Nat Funct Mol Chem, Xian, Shaanxi, Peoples R China.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
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2019 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 11, no 6, p. 6448-6455Article in journal (Refereed) Published
Abstract [en]

This paper reports a procedure leading to shear exfoliation of pristine few-layer graphene flakes in water and subsequent site-selective formation of Cu/graphene films on polymer substrates, both of which are enabled by employing the water soluble 1-pyrenebutyric acid tetrabutylammonium salt (PyB-TBA). The exfoliation with PyB-TBA as an enhancer leads to as-deposited graphene films dried at 90 °C that are characterized by electrical conductivity of ∼110 S/m. Owing to the good affinity of the tetrabutylammonium cations to the catalyst PdCl42–, electroless copper deposition selectively in the graphene films is initiated, resulting in a self-aligned formation of highly conductive Cu/graphene films at room temperature. The excellent solution-phase and low-temperature processability, self-aligned copper growth, and high electrical conductivity of the Cu/graphene films have permitted fabrication of several electronic circuits on plastic foils, thereby indicating their great potential in compliant, flexible, and printed electronics.

Place, publisher, year, edition, pages
2019. Vol. 11, no 6, p. 6448-6455
Keywords [en]
graphene, electroless copper deposition, solution-phase processing, self-aligned metallization, flexible electronics
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-378999DOI: 10.1021/acsami.8b21162ISI: 000459221900096PubMedID: 30656938OAI: oai:DiVA.org:uu-378999DiVA, id: diva2:1297248
Funder
Swedish Foundation for Strategic Research , Dnr SE13-0061Swedish Research Council, 621-2014-5596Available from: 2019-03-19 Created: 2019-03-19 Last updated: 2019-04-08Bibliographically approved
In thesis
1. Solution-Processable Conductive Graphene-Based Materials for Flexible Electronics
Open this publication in new window or tab >>Solution-Processable Conductive Graphene-Based Materials for Flexible Electronics
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis work explores electrical conductors based on few-layer graphene flakes as an enabler for low-cost, mechanically flexible, and high-conductivity conductors in large area flexible and printed electronic devices. The flakes are deposited from aqueous solutions and processed at low temperature.

Graphene is selected for its excellent properties in mechanical, optical, electronic, and electrical aspects. However, thin films of pristine few-layer graphene flakes deposited from dispersions normally exhibit inferior electrical conductivity. One cause responsible for this problem is the loose stacking and random orientation of graphene flakes in a graphene deposition. We have solved this problem by implementing a simple post-deposition treatment leading to dramatically densified and planarized thin films. Significantly increased electrical conductivity by ~20 times is obtained. The 1-pyrenebutyric acid tetrabutylammonium salt as an exfoliation enhancer and dispersant in water yields ~110 S/m in conductivity when the graphene based thin films are processed at 90 °C. In order to achieve higher conductivity, a room-temperature method for site-selective copper electroless deposition has been developed. This method is of particular interest for the self-aligned copper deposition to the predefined graphene films. The resultant two-layer graphene/copper structure is characterized by an overall conductivity of ~7.9 × 105 S/m, an increase by ~7000 times from the template graphene films. Several electronic circuits based on the graphene/copper bilayer interconnect have been subsequently fabricated on plastic foils as proof-of-concept demonstrators. Alternatively, highly conductive composites featuring graphene flakes coated with silver nanoparticles with electrical conductivity beyond 106 S/m can be readily obtained at 100 oC. Moreover, a highly conductive reduced-graphene-oxide/copper hybrid hydrogel has been achieved by mixing aqueous graphene oxide solution and copper-containing Fehling's solution. The corresponding aerogel of high porosity exhibits an apparent electrical conductivity of ~430 S/m and delivers a specific capacity of ~453 mAh g−1 at current density of 1 A/g. The experimental results presented in this thesis show that the solution-phase, low-temperature fabrication of highly conductive graphene-based materials holds promises for flexible electronics and energy storage applications. 

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2019. p. 65
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1799
Keywords
Graphene, Graphene oxide, Silver, Copper, Composite, Conductive inks, Flexible electronics, Printed electronics
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Research subject
Engineering Science with specialization in Electronics
Identifiers
urn:nbn:se:uu:diva-381348 (URN)978-91-513-0636-0 (ISBN)
Public defence
2019-06-12, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen. 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2019-05-13 Created: 2019-04-08 Last updated: 2019-06-18

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Zhao, JieWen, ChenyuSun, RuiZhang, Shi-LiZhang, Zhi-Bin

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