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ISSN 1822-508X

KAUNAS UNIVERSITY OF TECHNOLOGY

VYTAUTAS MAGNUS UNIVERSITY

LITHUANIAN ENERGY INSTITUTE

RIGA TECHNICAL UNIVERSITY

HYDROGEN ENERGY ASSOCIATION

4

rd

International Conference

RADIATION INTERACTION WITH MATERIAL

AND ITS USE IN TECHNOLOGIES 2012

Kaunas, Lithuania

May 14-17, 2012

Program and materials

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Executive editor A. Grigonis

Conference is organized by:

Kaunas University of Technology Hydrogen Energy Association

Vytautas Magnus University Lithuanian Energy Institute

Riga Technical University Sumy State University

Programme Committee A. Grigonis (Lithuania) V. Anishchik (Belarus) R. Andrievski (Russia) J. Dudonis (Lithuania) A. Galdikas (Lithuania) D. H. Gregory (Scotland, UK) F. Komarov (Belarus) R. Letfullin (USA) G. Laukaitis (Lithuania) H. Manikowski (Poland) A. Medvid (Latvia) E. Mellikov (Estonia) D. Milius (Lithuania) H. Mimura (Japan) A. Pogrebnjak (Ukraine) L. Praneviius (Lithuania) S. Tamuleviius (Lithuania) C. Templier (France) E. Ušpuras (Lithuania) J. V. Vaitkus (Lithuania) J. Žuk (Poland) P. Žukowski (Poland) Organizing Committee

G. Laukaitis (Lithuania) - chairman R. Naujokaitis (Lithuania) B. Abakeviien (Lithuania) V. Vincinait (Lithuania) L. Anceviien (Lithuania) L. Puodžiukynas (Lithuania) L. Vigricait (Lithuania) Ž. Rutknien (Lithuania) L. Marcinauskas (Lithuania) Editorial Committee A. Grigonis (Lithuania) G. Laukaitis (Lithuania) L.L. Praneviius (Lithuania) A. Galdikas (Lithuania) M. Šilinskas (Germany) B. Vengalis (Lithuania) R. Naujokaitis (Lithuania) P. Onufrijevs (Latvia)

Conference is supported by:

The European Social Fund Agency Hydrogen energy association

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P4-13

INFLUENCE OF ULTRASONIC RADIATION ON

THE AMORPHOUS ZEOLITE – PORTLAND

CEMENT SYSTEM

L. Jakeviius

1a

, D. Vaiiukynien

1b

, A. Demenko

2

1a

Department of Physics, bFaculty of Chemical Technology; Kaunas University of Technology, Kaunas [Lithuania]. 2Department of Engineering Technology; University of Twente, Enschede [Netherlands]

Department of Physics, Kaunas University of Technology, Studentu str. 50, LT-51368 Kaunas, Lithuania; E-mail: danute.palubinskaite@ktu.lt

Abstract

This paper considers the investigation of influence of an amorphous synthetic

zeolite with inserted Ca2+ ions additive (ASZ) on the hydration temperature of Portland

cement paste.In this investigation the sonicated Portland cement paste is compared to

the non-sonicated paste; and then the cement paste hydration process is analyzed by the means of temperature measurements. The temperature measurement results confirm that the sonication process accelerates the exothermic chemical reaction between the Portland cement and water.

Keywords: cement hydration, amorphous zeolite, ultrasonic radiation, sonication

Nowadays, there is much discussion concerning incorporation of natural and synthetic zeolites in blended cements [1–3]. Therefore, applications of blended cements, instead of ordinary Portland cement, are increasing rapidly in the industry.

In the reported study [4] a sonication process is applied by means of which a deagglomeration of larger particles of densified silica fume is achieved. This treatment enabled to increase quantity of submicrometric particles in samples. The effect of sonication process on densified silica fumeproduces a greater quantity of very fine particles, which improves the pozzolanic reactivity of silica fume and increases fixation of hydrated lime. This behavior also enables to achieve a higher mechanical strength in mortars which are produced with sonicated silica fume.

Silica fumes are subjected to ultrasonic treatment in order to decrease particle agglomeration and improve particle dispersion. The effectiveness of the sonication is observed as a reduction in particle size distribution of the sonicated silica fume (SSF) compared to the non-sonicated silica fume. SSF is added to Portland cement, and then the hydrated paste is analysed. Micro-structural characterization results show an increase in the reactivity of the silica fume after the treatment [5].

Uniform dispersion of carbon nanotubes is mandatory, and a sonication technique is adapted to disperse them [6]. Another method used for dispersion

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of carbon nanotubes [7,8] is based on the sonication of ordinary Portland cement and carbon nanotubes simultaneously.

The paper describes a new, powerful, patented piece of sonic equipment that operates in the low sonic frequency range, at 104 Hz, with nominal power of 75 kW. It has been tested for both physical and chemical sonic effects. A large-scale industrial application is described — the conditioning and pacification of ash from utility coal combustion by fluidized bed combustion. A variety of additional applications is suggested, most of which have been briefly tested [9].

In this study, the properties and the hydration process of Portland cement pastes containing synthetic amorphous zeolite are investigated. The Portland cement pastes with amorphous zeolite additive and without additive are subjected to ultrasonic treatment in order to increase the hydration rate of the cement paste. The Portland cement CEM I 52.R (mineral composition C3S = 50.7 %;

C2S = 18.5 %; C4AF = 14.2 %; C3A = 9.7 %) and amorphous synthetic zeolite

(ASZ) with inserted Ca2+ ions is used in this study. The investigated zeolite contains: Al2O3 = 23.3 %; SiO2 = 48.4 %; Na2O= 5.4 %; CaO = 5.6 %. The

compositions are varied by the contents of the ASZ addition: 0; 5; 10 and 15 %. The prepared cement pasta, placed in 90 mm diameter cylindrical chamber, was treated by ultrasonic radiation for 15 min. The ultrasonic radiation was generated using 28 kHz ultrasonic transducer of 60 W power. The X-ray powder diffraction data were collected employing DRON-6 X-ray diffractometer equipped with Bragg-Brentano geometry using Ni-filtered Cu K radiation and graphite monochromator. Operating voltage of 30 kV and emission current of 20 mA were used in the experiments. The chemical composition of the zeolite was determined by digests energy X-ray spectrometer (EDS) with a silicon-type detector (SD3). The cement paste hydration temperaturemeasurements were performed with 8-channel USB TC-08 Thermocouple Data Logger (temperature measurement range from -270 to 1820 °C).

ASZ was synthesized from sodium silicate and sodium aluminate solutions. The gel was formed immediately after mixing of solutions. The gel - ASZ was aged at room temperature for 72 hours. Ion exchange reactions were performed in the unstirred suspension: CaCl2 solution was filled up with

zeolite. The final product of the synthesis was filtered, dried at 60 °C temperature and sieved through a 0.5 mm mesh sieve. The measured X-ray diffraction patterns of the ASZ showed that it was in amorphous state (Fig. 1).

Experimental investigations show that ASZ affects temperature of hydration process in the cement paste (see Fig. 2, a). The results for pastes with 5; 10 and 15% additive are compared with pastes without the additive. This additive increases the maximum hydration temperature in all investigated cases. A higher hydration temperature accelerates the chemical reaction during which

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P4-13 0 10 20 30 40 50 60 70 0 500 1000 1500 2000 2500 2, deg. In te ns it y , a. u. C C C C CC C

Fig. 1. X-ray diffraction patterns of ASZ, where C is the calcite, a.u. are the arbitrary units,  is the diffraction angle.

a greater amount of heat is released. The highest hydration temperature is observed in specimens where 10% wt of ASZ additive is added. The test results show that ASZ additive at 10% and 15% of the cement paste accelerates the hydration process from 733 min (without the additive) to 633 min and 567 min, respectively. Moreover, it increased the maximum temperature of Portland cement hydration process by 6 °C and 1°C, respectively. Using 5% wt of ASZ additive, the cement paste changesthe hydration process duration very little, but the temperature maximum increases up to 3°C.

a b

Fig. 2. Cement paste hydration process temperature dependence on the quantity of amorphous zeolite additive: a) cement paste without ASZ (1) and with 5% (2), 10% (3)

and 15% (4) of zeolite and all samples are without sonication; b) cement paste without zeolite (1, 2) and with 5% of ASZ (3, 4); 1, 3 - before sonication and 2, 4 - after

sonication for 15 min.

The temperature measurement results show that the highest hydration process temperature is achieved after sonication for 15 min (sample 2 and 4) to compare with the control sample without sonication (sample 1 and 3). Moreover, the measurement results show that the highest hydration process

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temperature is achieved after sonication for 15 min (sample 2 and 4) to compare with the control sample without sonication (sample 1 and 3). The effectiveness of the sonication is observed as an increase in the maximum of hydration process temperature. One can conclude that the ASZ additive and sonication process accelerate the exothermic chemical reaction between the Portland cement and water.

References

1. Caputo D., Liguori B., Colella C. Some advances in understanding the pozzolanic activity of zeolites: The effect of zeolite structure. - Cement and Concrete Composites, 30, N5, 2008, 455-462 p.

2. Juengsuwattanan K., Seraphin S. Effects of Zeolite A on the Microstructure and Strength Development of Blended Cement. - Journal of the Microscopy Society of Thailand, N24(2), 2010, 94-98 p.

3. Ikotun B.D., Ekolu S. Strength and durability effect of modified zeolite additive on concrete properties. - Construction and Building Materials, 24, N5, 2010, 749-757 p.

4. Martinez-Velandia D., Paya J., Monzo J., Borrachero M. V.Effect of sonication on

the reactivity of silica fume in Portland cement mortars. - Advances in cement research, 23, N1, 2011, 23-31 p.

5. Erich D. Rodríguez, Lourdes Soriano, Jordi Payá, María Victoria Borrachero, José M. Monzó. Increase of the reactivity of densified silica fume by sonication treatment. - Ultrasonics Sonochemistry Available online 1 February 2012 In Press, Corrected Proof.

6. Manzur T., Yazdani N. Strength Enhancement of Cement Mortar with Carbon Nanotubes. Transportation Research Record.  Journal of the Transportation ResearchBoard.21,2010,102108p.

7. Makar J. M., Margeson J., Luh J. Carbon nanotube/cement composites-early results and potential applications. - Construction Materials. In Proceedings of ConMat’05 and Mindess Symposium, Vancouver, Canada, 22–24 August 2005, 32 p.

8. Makar J. M., Chan G. W., Growth of cement hydration products on single walled carbon nanotubes. - J. Am. Ceram. Soc., 92, 2009, 1303–1310 p.

9. Russell J. P. Scale-up of sonic energy for a major industrial application: ash conditioning for power utilities that use fluidized bed combustion. - Ultrasonics Sonochemistry, 7, 2000, 235–236 p.

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