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Particle generation by cosolvent spray pyrolysis: Effects of ethanol and ethylene glycol

Published online by Cambridge University Press:  06 August 2012

Kai Zhong ,
George Peabody ,
Howard Glicksman  and
Sheryl Ehrman
Kai Zhong
Affiliation:
Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland20742
George Peabody
Affiliation:
Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland20742
Howard Glicksman
Affiliation:
Department of Microcircuit Materials, DuPont Electronic Technologies, Research Triangle Park, North Carolina27709
Sheryl Ehrman*
Affiliation:
Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland20742
*
a)Address all correspondence to this author. e-mail: sehrman@eng.umd.edu
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Abstract

A cosolvent spray pyrolysis process was used for the generation of micrometer-sized pure copper particles. Ethylene glycol (EG) and ethanol (ET) were selected as cosolvents, and their effects on particle morphology and composition were systematically investigated. Experimental results showed that oxide-free copper particles could be generated at temperatures greater than 400 °C with either cosolvent. Hollow particles with cracks were generated with ET at temperatures from 400 to 1000 °C, whereas EG promoted the formation of porous particles at temperatures up to 600 °C and hollow shell particles with smooth surfaces at 875 and 1000 °C. Results from short residence time experiments indicated that, during the generation process, lamellar and fragment-like copper hydroxy nitrate [Cu2(OH)3NO3] precipitated when EG and ET were used respectively. Cu2(OH)3NO3 then decomposed to cupric oxide (CuO) and cuprous oxide (Cu2O). Finally the oxides were reduced to copper (Cu) in the reducing atmosphere created by EG and ET.

Type
Articles
Information
Journal of Materials Research , Volume 27 , Issue 19 , 14 October 2012 , pp. 2540 - 2550
Copyright
Copyright © Materials Research Society 2012

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References

REFERENCES

Brusic, V., Frankel, G.S., Roldan, J., and Saraf, R.: Corrosion and protection of a conductive silver paste. J. Electrochem. Soc. 142, 2591 (1995).CrossRefGoogle Scholar
Ohmi, T.: ULSI reliability through ultraclean processing. Proc. IEEE 81, 716 (2002).CrossRefGoogle Scholar
Songping, W. and Shuyuan, M.: Preparation of micron size copper powder with chemical reduction method. Mater. Lett. 60, 2438 (2006).CrossRefGoogle Scholar
Miki, H.: Method for producing copper powder. U.S. Patent No. 5 741 347, April 21, 1998.Google Scholar
Tani, H. and Ogata, N.: Production of copper powder. U.S. Patent No. 5 850 047, 1998.Google Scholar
Hosokura, T. and Maeda, A.: Method for producing the same and conductive paste. U.S. Patent No. 6 939 619, September 6, 2005.Google Scholar
Hao, G., Xu, Q., Han, F., Li, W., and Bai, S.: Processing and damping behavior of porous copper. Powder Metall. 52, 145 (2009).CrossRefGoogle Scholar
Champion, Y., Langlois, C., and Guerin, S.: Plasticity of copper with small grain size. Mater. Sci. Forum 482, 71 (2005).CrossRefGoogle Scholar
Chung, D.D.L.: Materials for thermal conduction. Appl. Therm. Eng. 21, 1593 (2001).CrossRefGoogle Scholar
Tsai, K.L. and Dye, J.L.: Nanoscale metal particles by homogeneous reduction with alkalides or electrides. J. Am. Chem. Soc. 113, 1650 (1991).CrossRefGoogle Scholar
Hirai, H., Nakao, Y., and Toshima, N.: Colloidal rhodium in poly(vinylpyrrolidone) as hydrogenation catalyst for internal olefins. Chem. Lett. 5, 545 (1978).CrossRefGoogle Scholar
Kurihara, L.K., Chow, G.M., and Schoen, P.E.: Nanocrystalline metallic powders and films produced by the polyol method. Nanostruct. Mater. 5, 607 (1995).CrossRefGoogle Scholar
Fievet, F., Fievetvincent, F., Lagier, J., Dumont, B., and Figlarz, M.: Controlled nucleation and growth of micrometer-size copper particles prepared by the polyol process. J. Mater. Chem. 3, 627 (1993).CrossRefGoogle Scholar
Cardenas-Trivino, G., Klabunde, K.J., and Dale, E.B.: Living colloidal palladium in nonaqueous solvents. Formation, stability, and film-forming properties. Langmuir 3, 986 (1987).CrossRefGoogle Scholar
Saton, N. and Kimura, K.: Metal colloids produced by means of gas evaporation technique. 5. Colloidal dispersion of Au fine particles to hexane, poor dispersion medium for metal sol. Bull. Chem. Soc. Jpn. 62, 1758 (1989).Google Scholar
Jain, S., Skamser, D.J., and Kodas, T.T.: Morphology of single-component particles produced by spray pyrolysis. Aerosol Sci. Technol. 27, 575 (1997).CrossRefGoogle Scholar
Majumdar, D., Shefelbine, T.A., Kodas, T.T., and Glicksman, H.D.: Copper (I) oxide powder generation by spray pyrolysis. J. Mater. Res. 11, 2861 (1996).CrossRefGoogle Scholar
Nagashima, K., Iwaida, T., Sasaki, H., Katatae, Y., and Kato, A.: Preparation of fine, spherical copper particles by spray pyrolysis technique. Nippon Kagaku Kaishi 1, 17 (1990).CrossRefGoogle Scholar
Jayanthi, G., Zhang, S., and Messing, G.: Modeling of solid particle formation during solution aerosol thermolysis: The evaporation stage. Aerosol Sci. Technol. 19, 478 (1993).CrossRefGoogle Scholar
Messing, G., Zhang, S., and Jayanthi, G.: Ceramic powder synthesis by spray-pyrolysis. J. Am. Chem. Soc. 76, 2707 (1993).Google Scholar
Stopic, S., Ilic, I., and Uskokovic, D.: Preparation of nickel submicron powder by ultrasonic spray pyrolysis. Int. J. Powder Metall. 32, 59 (1996).Google Scholar
Xia, B., Lenggoro, I., and Okuyama, K.: Preparation of Ni particles by ultrasonic spray pyrolysis of NiCl2• 6H2O precursor containing ammonia. J. Mater. Sci. 36, 1701 (2001).CrossRefGoogle Scholar
Gurmen, S., Guven, A., Ebin, B., Stopic, S., and Friedrich, B.: Synthesis of nano-crystalline spherical cobalt-iron (Co-Fe) alloy particles by ultrasonic spray pyrolysis and hydrogen reduction. J. Alloys Compd. 481, 600 (2009).CrossRefGoogle Scholar
Biskos, G., Vons, V., Yurteri, C.U., and Schmidt-Ott, A.: Generation and sizing of particles for aerosol-based nanotechnology. Kona Powder Part. J. 26, 13 (2008).CrossRefGoogle Scholar
Gurav, A., Kodas, T., Pluym, T., and Xiong, Y.: Aerosol processing of materials. Aerosol Sci. Technol. 19, 411 (1993).CrossRefGoogle Scholar
Kim, J.H., Babushok, V.I., Germer, T.A., Mulholland, G.W., and Ehrman, S.H.: Cosolvent-assisted spray pyrolysis for the generation of metal particles. J. Mater. Res. 18, 1614 (2003).CrossRefGoogle Scholar
Firmansyah, D.A., Kim, T., and Kim, S.: Crystalline phase reduction of cuprous oxide (Cu2O) nanoparticles accompanied by a morphology change during ethanol-assisted spray pyrolysis. Langmuir 25, 7063 (2009).CrossRefGoogle ScholarPubMed
Kim, J., Rodriguez, J., Hanson, J., Frenkel, A., and Lee, P.: Reduction of CuO and Cu2O with H-2: H embedding and kinetic effects in the formation of suboxides. J. Am. Chem. Soc. 125, 10684 (2003).CrossRefGoogle ScholarPubMed
Kim, J.H., Germer, T.A., and Mulholland, G.W.: Size-monodisperse metal nanoparticles via hydrogen-free spray pyrolysis. J. Appl. Phys. 36, L714 (1997).Google Scholar
Okuyama, K. and Lenggoro, I.W.: Preparation of nanoparticles via spray route. Chem. Eng. Sci. 58, 537 (2003).CrossRefGoogle Scholar
Speight, J.: Lange’s Handbook of Chemistry, 70th Anniversary Edition, 16th ed. (McGraw-Hill Professional, New York, NY, 2004); pp. 384–385, Section 2.Google Scholar
(NFPA) NFPA: NFPA 704: Standard System for the Identification of the Hazards of Materials for Emergency Response (NFPA, Quincy, MA, 2007).Google Scholar
Zhon, K., Peabody, G., Glicksman, H., Marshall, A.W., and Ehrman, S.: Atomization behavior of copper nitrate solution in 1.7 MHz ultrasonic nebulizer (2012, unpublished).Google Scholar
McCusker, L.B., Von Dreele, R.B., Cox, D.E., Louer, D., and Scardi, P.: Rietveld refinement guidelines. J. Appl. Crystallogr. 32, 36 (1999).CrossRefGoogle Scholar
Widiyastuti, W., Wang, W.N., Lenggoro, I.W., Iskandar, F., and Okuyama, K.: Simulation and experimental study of spray pyrolysis of polydispersed droplets. J. Mater. Res. 22, 1888 (2007).CrossRefGoogle Scholar
Lvov, B. and Novichikhin, A.: Mechanism of thermal decomposition of hydrated copper nitrate in vacuo. Spectrochim. Acta, Part B 50, 1459 (1995).CrossRefGoogle Scholar
Jackson, J., Fonseca, R., and Holcombe, J.: Mass spectral studies of thermal decomposition of metal nitrates. Spectrochim. Acta, Part B 50, 1449 (1995).CrossRefGoogle Scholar
Park, S. and Lee, C.E.: Layered copper hydroxide n-alkylsulfonate salts: Synthesis, characterization, and magnetic behaviors in relation to the basal spacing. J. Phys. Chem. B 109, 1118 (2005).CrossRefGoogle Scholar
Pruppacher, H.R. and Klett, J.D.: Microphysics of Clouds and Precipitation, 2nd ed. (Springer-Verlag, New York, 1996); pp. 502–561, Chap. 13.Google Scholar
Friedlander, S.K.: Smoke, Dust, and Haze: Fundamentals of Aerosol Behavior (John Wiley & Sons, New York, 1977); pp. 50–88, Chap. 3.Google Scholar