Abstract
Flame synthesis is one of the most versatile and promising technologies for large-scale production of nanoscale materials1,2,3. Pyrolysis has recently been shown to be a useful route for the production of single-walled nanotubes4, quantum dots5 and a wide variety of nanostructured ceramic oxides for catalysis6 and electrochemical applications7. An understanding of the mechanisms of nanostructural growth in flames has been hampered by a lack of direct observations of particle growth8,9,10,11,12,13,14,15,16,17,18,19,20,21, owing to high temperatures (2,000 K), rapid kinetics (submillisecond scale), dilute growth conditions (10−6 volume fraction) and optical emission of synthetic flames. Here we report the first successful in situ study of nanoparticle growth in a flame using synchrotron X-ray scattering. The results indicate that simple growth models, first derived for colloidal synthesis22, can be used to facilitate our understanding of flame synthesis. Further, the results indicate the feasibility of studies of nanometre-scale aerosols of toxicological23 and environmental24 concern.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Friedlander, S.K. Smoke, Dust, and Haze: Fundamentals of Aerosol Dynamics 2nd edn (Oxford Univ. Press, New York, 2000).
Ulrich, G.D. Flame synthesis of fine particles. Chem. Eng. News 62, 22–29 (1984).
Pratsinis, S.E. Flame aerosol synthesis of ceramic powders. Prog. Energy Combust. Sci. 24, 197–219 (1998).
Van der Wal, R.L., Berger, G.M. & Hall, L.J. Single-walled carbon nanotube synthesis via a multi-stage flame configuration. J. Phys. Chem. B 106, 3564–3567 (2002).
Madler, L., Stark, W.J. & Pratsinis, S.E. Rapid synthesis of stable ZnO quantum dots. J. Appl. Phys. 92, 6537–6540 (2002).
Stark, W.J., Pratsinis, S.E. & Baiker, A. Flame made titania/silica epoxidation catalysts. J. Catal. 203, 516–524 (2001).
Madler, L., Stark, W.J. & Pratsinis, S.E. Flame-made ceria nanoparticles. J. Mater. Res. 17, 1356–1362 (2002).
Anala, S. et al. In situ NMR spectroscopy of combustion. J. Am. Chem. Soc. 125, 13298–13302 (2003).
Tsantilis, S., Briesen, H. & Pratsinis, S.E. Sintering time for silica particle growth. Aerosol Sci. Technol. 34, 237–246 (2001).
Arabi-Katbi, O.I., Pratsinis, S.E., Morrison, P.W. Jr & Megaridis, C.M. Monitoring the flame synthesis of TiO2 particles by in-situ FTIR spectroscopy and thermophoretic sampling. Combust. Flame 124, 560–572 (2001).
Morrison, P.W., Raghavan, R., Timpone, A.J., Artelt, C.P. & Pratsinis, S.E. In situ Fourier transform infrared characterization of the effect of electrical fields on the flame synthesis of TiO2 particles. Chem. Mater. 9, 2702–2708 (1997).
Dobbins, R.A. & Megaridis, C.M. Morphology of flame-generated soot as determined by thermophoretic sampling. Langmuir 3, 254–259 (1987).
Köylü, Ü.Ö., McEnally, C.S., Rosner, D.E. & Pfefferle, L.D. Simultaneous measurements of soot volume fraction and particle size / microstructure in flames using a thermophoretic sampling technique. Combust. Flame 110, 494–507 (1997).
Hurd, A.J. & Flower, W.L. In situ growth and structure of fractal silica aggregates in a flame. J. Colloid Interface Sci. 122, 178–192 (1988).
Xing, Y., Köylü, Ü.Ö. & Rosner, D.E. In situ light-scattering measurements of morphologically evolving flame-synthesized oxide nanoaggregates. Appl. Opt. 38, 2686–2697 (1999).
King, G.B., Sorensen, C.M., Lester, T.W. & Merklin, J.F. Direct measurements of aerosol diffusion constants in the intermediate Knudsen regime. Phys. Rev. Lett. 50, 1125–1128 (1983).
Chowdhury, D.P., Sorensen, C.M., Taylor, T.W., Merklin, J.F. & Lester, T.W. Application of photon correlation spectroscopy to flowing brownian motion systems. Appl. Opt. 23, 4149–4154 (1984).
Taylor, T.W. & Sorensen, C.M. Gaussian beam effects on the photon correlation spectrum from a flowing brownian motion system. Appl. Opt. 25, 2421–2426 (1986).
Sorensen, C.M., Hageman, W.B., Rush, T.J., Huang, H. & Oh, C. Aerogelation in a flame soot aerosol. Phys. Rev. Lett. 80, 1782–1785 (1998).
Sorensen, C.M., Hagemann, W.B. Two-dimensional soot. Langmuir 17, 5431–5434 (2001).
Zachariah, M.R. & Semerjian, H.G. Simulation of ceramic particle formation: Comparison with in-situ measurements. Am. Inst. Chem. Eng. J. 35, 2003–2012 (1989).
Sugimoto, T. Monodisperse Particles (Elsevier, New York, 2001).
Pyne, S. Small particles add up to big disease risk. Science 295, 1994 (2002).
Chameides, W.L. & Bergin, M. Soot takes center stage. Science 297, 2214–2215 (2002).
Guinier, A. & Fournet, G. Small Angle Scattering of X-rays (John Wiley & Sons, New York, 1955).
Glatter, O. & Kratky, O. Small-angle X-ray Scattering (Academic, London, 1982).
Roe, R.-J. Methods of X-Ray and Neutron Scattering in Polymer Science (Oxford Univ. Press, New York, 2000).
Beaucage, G., Kammler, H.K. & Pratsinis, S.E. Estimate of particle-size polydispersity from small-angle scattering. J. Appl. Crystallogr. (in the press).
Beaucage, G. Approximations leading to a unified exponential/power-law approach to small-angle scattering. J. Appl. Crystallogr. 28, 717–728 (1995).
Beaucage, G. Small-angle scattering from polymeric mass fractals of arbitrary mass-fractal dimension. J. Appl. Crystallogr. 29, 134–146 (1996).
Hyeon-Lee, J., Beaucage, G., Pratsinis, S.E. & Vemury, S. Fractal analysis of flame-synthesized nanostructured silica and titania powders using small-angle X-ray scattering. Langmuir 14, 5751–5756 (1998).
Kammler, H.K., Beaucage, G., Mueller, R. & Pratsinis, S.E. Structure of flame-made silica nanoparticles by ultra small-angle x-ray scattering. Langmuir 20, 1915–1921 (2004).
Pontoni, D., Narayanan, T. & Rennie, A.R. Time-resolved SAXS study of nucleation and growth of silica colloids. Langmuir 18, 56–59 (2002).
Acknowledgements
This work was supported by the US National Science Foundation (CTS-0070214), the Swiss National Science Foundation (200021-101901/1), the Swiss Commission for Technology and Innovation (TopNano21-5487.1) and the synchrotron facilities at ESRF (beam time allocation ME421). We thank J. Gorini for technical assistance; we also thank D. J. Kohls (at the University of Cincinnati), and J. Ilavsky and P. Jemian (at UNICAT, Advanced Photon Source) for collaborative work. G.B. thanks the University of Cincinnati for sabbatical leave at ETH Zentrum.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Rights and permissions
About this article
Cite this article
Beaucage, G., Kammler, H., Mueller, R. et al. Probing the dynamics of nanoparticle growth in a flame using synchrotron radiation. Nature Mater 3, 370–373 (2004). https://doi.org/10.1038/nmat1135
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nmat1135
This article is cited by
-
In-situ aerosol nanoparticle characterization by small angle X-ray scattering at ultra-low volume fraction
Nature Communications (2019)
-
In situ observation of synthesized nanoparticles in ultra-dilute aerosols via X-ray scattering
Nano Research (2019)
-
Electric field effects on the growth of flame-synthesized nanosilica: a two-stage modeling
Journal of the Iranian Chemical Society (2019)
-
Ultra-Small-Angle X-ray Scattering Instrument at the Advanced Photon Source: History, Recent Development, and Current Status
Metallurgical and Materials Transactions A (2013)
-
Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight
Nature (2012)