Supercritical Hydrothermal Synthesis of Polyacrylic Acid-Capped Copper Nanoparticles and Their Feasibility as Conductive
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https://doi.org/10.1007/s11664-020-08370-w Ó 2020 The Minerals, Metals & Materials Society
Supercritical Hydrothermal Synthesis of Polyacrylic Acid-Capped Copper Nanoparticles and Their Feasibility as Conductive Nanoinks NANAMI NUMAGA,1 HIROMICHI HAYASHI and RICHARD L. SMITH JR.1,3,5
,2,4
1.—Graduate School of Environmental Studies, Tohoku University, Aramaki Aza Aoba 6-611, Aoba-ku, Sendai 980-8579, Japan. 2.—Research Institute for Chemical Process Technology, National Institute of Advanced Industrial Science and Technology, 4-2-1, Nigatake, Miyagino-ku, Sendai 983-8551, Japan. 3.—Research Center of Supercritical Fluid Technology, Tohoku University, Aramaki Aza Aoba 6-6-11, Aoba-ku, Sendai 980-8579, Japan. 4.—e-mail: [email protected]. 5.—e-mail: [email protected]
Polyacrylic acid (PAA) applied as surface modifier of zero-valent copper nanoparticles (CuNPs) for electronic printing inks has great potential to replace presently used polymers, because of its favorable technical, environmental and biodegradability characteristics. Continuous synthesis (400°C, 30 MPa) of nanoparticles in supercritical water with short reaction times (1.1 s) was used to form PAA-surface-modified zero-valent (34–46 nm) CuNPs. CuNP particle sizes decreased with an increase in PAA molecular mass (5000, 25,000) and were stable as dispersions in methanol and 1-propanol, respectively. The resistivity of conductive films prepared with CuNPs decreased with an increase in heating temperature. The minimum resistivity of the PAAmodified CuNPs was 1.4 9 105 X cm at 320°C (PAA25000) and 4.2 9 104 X cm at 350°C (PAA5000), demonstrating the feasibility of PAA as a dispersant and surface modifier for CuNPs. Polyacrylic acid is thus effective as a surface modifier for zero-valent metal nanoparticles and expands the possible applications in sustainable printed electronics. Key words: Nanotechnology, copper nanoparticles, electronic printing, polymer dispersant
INTRODUCTION Printed electronics are being explored worldwide due to their potential use in functional low-cost devices that are flexible, stretchable, and lightweight.1 An electrical transmission line is formed by deposition of a conductive ink onto a substrate, followed by sintering. Printed electronic methods are environmentally benign, have low material and processing waste and require only two steps for conductive line formation compared with present multi-step methods.2 Conductive inks made from
(Received January 23, 2020; accepted July 29, 2020)
Au and Ag have been proposed and are widely used, although both of these metals are expensive, and Ag is problematic for electrical migration that tends to lead to dendrite growth and short circuits.3,4 Copper nanoinks have been noted as an alternative to Au or Ag for the production of conductive lines, owing to their cost-effectiveness and favorable environmental properties.5 Copper nanoparticles (CuNP) have been synthesized by various methods, including sol– gel,6 reverse-micelle,7 thermal decomposition,8 polyol,9 and supercrit
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