Geopolymers
Inorganic polymeric new materials
Author:
Author:
Uwe Burghaus
Uwe Burghaus
Department of Chemistry and Biochemistry, North Dakota State University, Fargo, ND, 58108, USA
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Abstract
The effect of carbon nanotubes’ (CNT) crystal structure on chemical reactivity has been studied in much detail in the liquid phase using CNT suspension. This type of information is pertinent for developing CNT separation strategies. However, few experimental studies are available providing data for gas–CNT interactions utilizing ultra-high vacuum (UHV) surface science techniques. Structure–activity relationships (SAR) for gas–surface interactions are important for sensor designs and heterogeneous catalysis exploring, for example, CNT’s potential as a support for fuel cell catalysts. We report on UHV kinetics experiments with single-wall metallic, semiconducting, and mixed CNTs in order to provide the experimental basis to correlate CNT’s crystal structure and chemical activity. Thermal desorption spectroscopy (TDS), a simple temperature ramping technique, has been used to determine the binding energies of a number of probe molecules including alkanes, alcohols, thiophene, benzene, and water on CNTs at UHV conditions. TDS allows for the identification of adsorption sites of probe molecules in CNT bundles, using gold foil or silica as a support for the drop-and-dry technique. A weak and probe molecule dependent SAR is present for adsorption inside the CNTs but not for the population of external sites by the probe molecules. The experimental data are in part consistent with current theoretical predictions by other groups. In addition, the effect of different solvents (methanol, SDS, and NMP) and cleaning procedures will briefly be discussed using results of spectroscopic (Auger electron spectroscopy) and kinetic techniques. Furthermore, molecular beam scattering techniques were utilized to characterize the adsorption dynamics, i.e., the gas-to-surface energy transfer processes of alkanes on CNTs. For example, opening the CNT tube ends by high temperature annealing, increases the so-called initial adsorption probability, that is, the probability for adsorption in the limit of zero surface concentration (coverage). This result directly illustrates the effect of large surface areas of CNTs, using internal and external surfaces, for gas adsorption.
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1. Komarneni, M, Sand, A, Goering, J, Burghaus, U. Adsorption kinetics of methanol in carbon nanotubes revisited—solvent effects and pitfalls in ultra-high vacuum surface science experiments. Chem Phys Lett. 2009;473:131–137. .
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2. Funk, S, Hokkanen, B, Nurkig, T, Burghaus, U, White, B, O’Brien, S, Turro, N. Adsorption dynamics and kinetics of alkanes on carbon nanotubes. J Phys Chem C. 2007;111:8043–8047. .
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3. Komarneni, M, Sand, A, Lu, M, Burghaus, U. Adsorption kinetics of small organic molecules on thick and thinner layers of carbon nanotubes. Chem Phys Lett. 2009;470:300–304. .
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4. Burghaus, U, Bye, D, Cosert, K, Goering, J, Guerard, A, Kadossov, E, Lee, E, Madoyama, Y, Richter, N, Schaefer, E, Smith, J, Ulness, D, Wymor, D. Methanol adsorption in carbon nanotubes. Chem Phys Lett. 2007;442:344–348. .
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5. Goering, J, Kadossov, E, Burghaus, U. Adsorption kinetics of alcohols on single wall carbon nanotubes—an ultra-high vacuum surface chemistry study. J Phys Chem C. 2008;112:10114–10119. .
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6. Komarneni, M, Sand, A, Goering, J, Burghaus, U, Lu, M, Veca, M, Sun, YP. Possible effect of carbon nanotube diameter on gas-surface interactions—the case of benzene, water, and n-pentane adsorption on SWCNTs at ultra-high vacuum conditions. Chem Phys Lett. 2009;476:227–231. .
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7. Goering J , Burghaus U. Adsorption kinetics of thiophene on single-walled carbon nanotubes (CNTs). Chem Phys Lett. 2007;447:121–5.
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8. Funk, S, Goering, J, Burghaus, U. Adsorption kinetics of small organic molecules on a silica wafer: butane, pentane, nonane, thiophene, and methanol adsorption on SiO2/Si(111). Appl Surf Sci. 2008;254:5271–5276. .
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9. Funk, S, Nurkic, T, Burghaus, U. Reactivity screening of silica. Appl Surf Sci. 2007;253:4860–4865. .
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10. Kadossov, E, Goering, J, Burghaus, U. Adsorption of linear and branched alkanes on HOPG: a molecular beam scattering study. Surf Sci. 2007;601:3421–3424. .
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11. Bronikowski, MJ, Willis, PA, Colbert, DT, Smith, KA, Smalley, RE. Gas-phase production of carbon single-walled nanotubes from carbon monoxide via the HiPco process: a parametric study. J Vac Sci Technol A. 2001;19:1800–1804. .
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12. Burghaus U . Gas-carbon nanotubes interactions: a review of surface science studies on CNTs, in carbon nanotubes—Research trends, New York: Nova Science; 2009. ISBN 978-1-60692-236-1.
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13. Kondratyuk, P, Wang, Y, Johnson, JK, Yates, JT. Observation of a one-dimensional adsorption site on carbon nanotubes: adsorption of alkanes of different molecular length. J Phys Chem B. 2005;109:20999–21003. .
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14. Funk, S, Hokkanen, B, Burghaus, U, Ghicov, A, Schmuki, P. Unexpected adsorption of oxygen on TiO2 nanotube arrays—influence of crystal structure. Nano Lett. 2007;7:1091–1095. .
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15. Funk S , Hokkanen B, Nurkic T, Goering J, Kadossov E, Burghaus U, Ghicov A, Schmuki P, Yu ZQ, Thevuthasan S, Saraf LV. Reactivity screening of anatase TiO2 nanotube arrays and anatase thin films: a surface chemistry point of view, ACS Symposium series 996, Chicago: Oxford University Press; ISBN 978-0-8412-6969-9.
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16. Hokkanen, B, Funk, S, Burghaus, U, Ghicov, A, Schmuki, P. Adsorption kinetics of alkanes on TiO2 nanotubes array—structure-activity relationship. Surf Sci. 2008;601:4620–4624. .
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17. Komarneni, M, Sand, A, Nevin, P, Zak, A, Burghaus, U. Adsorption and reaction kinetics of small organic molecules on WS2 nanotubes: an ultra-high vacuum study. Chem Phys Lett. 2009;479:109–113. .
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18. Linsebigler, A, Lu, Gu, Yates, JT. CO chemisorption on TiO2(110): oxygen vacancy site influence on CO adsorption. J Chem Phys. 1995;103:9438–9444. .
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19. King, DA, Wells, MG. Molecular beam investigation of adsorption kinetics on bulk metal targets: nitrogen on tungsten. Surf Sci. 1972;29:454 .
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| Journal of Thermal Analysis and Calorimetry | |
|---|---|
| Language | English |
| Size | A4 |
| Year of Foundation |
1969 |
| Volumes per Year |
1 |
| Issues per Year |
24 |
| Founder | Akadémiai Kiadó |
| Founder's Address |
H-1117 Budapest, Hungary 1516 Budapest, PO Box 245. |
| Publisher | Akadémiai Kiadó Springer Nature Switzerland AG |
| Publisher's Address |
H-1117 Budapest, Hungary 1516 Budapest, PO Box 245. CH-6330 Cham, Switzerland Gewerbestrasse 11. |
| Responsible Publisher |
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| ISSN | 1388-6150 (Print) |
| ISSN | 1588-2926 (Online) |
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Temperature dependence of the rate of reaction in thermal analysis
The Arrhenius equation in condensed phase kinetics
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