ࡱ> hjcdefg`pbjbjss @I3%>****RRRDDKDKDK8|KL<LoL:L"MMMUUUwnynynynynynyn$phJsniRUUSUUUn**MMQohhhUZ *MRMwnhUwnhhkTRkML |{-|DK_&kcmo0Lok,s"eskksRkpU/Uh=U IUYUUUnnfUUULoUUUU<<<D$<<<<<fZ****** HYDRATION STUDY OF ORDINARY PORTLAND CEMENT IN THE PRESENCE OF LEAD(II) OXIDE Damir Barbir*, Pero Dabi, Petar Krolo Department of Inorganic Technology, Faculty of Chemistry and Technology, University of Split, Teslina 10, 21000 Split, Croatia * Corresponding autor: Damir Barbir Tel. +385 21 329 441; fax: +385 21 329 461 E-mail address:  HYPERLINK "mailto:dbarbir@ktf-split.hr" dbarbir@ktf-split.hr Other authors: Pero Dabi Tel. +385 21 329 441; fax: +385 21 329 461 E-mail address:  HYPERLINK "mailto:dbarbir@ktf-split.hr" dabic@ktf-split.hr Petar Krolo Tel. +385 21 329 470; fax: +385 21 329 461 E-mail address:  HYPERLINK "mailto:dbarbir@ktf-split.hr" krolo@ktf-split.hr Abstract The aim of this work is to investigate the effect of the addition of lead(II) oxide on hydration heat and specific conductivity of a CEM I Portland cement. The measurements were made at 20 oC, defined water/solid ratio, W/S = 0.5 and different contents of lead(II) oxide (0 1 wt. %). The heats production during hydration were determined by differential microcalorimetry up to 48 hours of hydration and the specific conductivity by a digital conductometer. Thermal gravimetric analysis (TGA) was employed in the characterization of the cement structure. The hydration heat results show that the addition of lead(II) oxide affect the cement hydration kinetics. Kinetic curves show that higher content of lead(II) oxide slow down the hydration processes and the heat values are lower. Addition of lead(II) oxide significantly delays the time appearance of the maximum conductivity. Setting time is prescribed by standard for a particular type of cement and can be determined based on the appearance of specific conductivity maximum, which occurs at the setting time. Acceptable share of lead(II) oxide is the one at which time the appearance of the conductivity maximum permitted standard limits. It was found that the acceptable amount of lead (II) oxide in cement system is w = 0,25 wt. %. Keywords: Stabilization/solidification (S/S), Hydration heat, Specific conductivity, Differential microcalorimetry, Thermogravimetric analysis (TGA) 1. Introduction Solidification/stabilization (S/S) is a technique for immobilizing hazardous wastes in binding materials, mostly cement-based, to delay the release of toxic components to the environment. Waste material is often S/S treated and is then landfilled or recycled into new building materials [1-3]. Among metal wastes, those containing Pb represents a serious issue. Pb derivatives are employed in mining and metallurgic industries, manufacture of coating pigments, imprint and typographer and plastic incineration. In humans, Pb exposure can lead to a wide range of biological effects depending on the level and duration of exposure. High levels of exposure may result in toxic biochemical effects in humans which in turn cause problems in the synthesis of haemoglobin, effects on the kidneys, gastrointestinal tract, joints and reproductive system [4]. Ordinary Portland cement (OPC) is often used as the binding agent on its own, or in combination with cement replacement materials, which may be hydraulic (cement kiln dust) or pozzolanic (pulverized fuel ash, slag etc.) in nature [5]. A great number of studies investigated the effect of lead on the hydration of cement phases. Lead retards the setting of cement due to the formation of compounds which cover the silicate phases. Glasser [6] reported that calcium silicate hydrates (C S H) and calcium sulfoaluminate hydrates are largely responsible for the retention of Pb. Using X-ray diffraction Hamilton et al [7] do not identify any lead compounds in cement/lead oxide system after a 28-day curing time and they concluded that lead compounds in cement matrices are amorphous. Tashiro et al reported that common hydration products are formed during the hydration of C3A in the presence of PbO. But it decreases the compressive strength of C3A [8]. In the present study, a PbO was solidified and stabilized by different proportion of OPC. This work has examined the effect of PbO on hydration processes using differential microcalorimetry, conductometry and TG analysis. The main task of this study is to determine an acceptable amount of PbO in the cement system for its successful stabilization and solidification. 2. Experimental 2.1. Materials and sample preparation All the measurements were carried on using OPC and different content of lead(II) oxide. OPC (according to EN-197 CEM I) was obtained from CEMEX Croatia cement plant (Kaatel Suurac, Croatia). Its chemical composition and physical properties are shown in Table 1 and 2. Lead(II) oxide, PbO, p.a., was obtained from P.P.H. Polskie Odezynniki Chem-Gliwice, Poland. Samples for microcalorimetrical measurements were prepared by mixing cement and 0 - 1 wt. % of PbO. The total mass of the solid sample was constant and it was 4 g. A water to solid ratio of 0.5 was used for all mixes and measurements were carried out at a temperature of 20 oC. Samples for conductometrical measurements were prepared in the same way as the samples for microcalorimetrical measurements, exept the total mass of the solid sample was 100 g. Cement pastes for TG analysis were hydrated 28 days in a thermostat at a temperature of 20 oC. After this curing time they were ground and sieved through a standard 4900 mesh/cm2 sieve. Table 1 here Table 2 here 2.2. Methods 2.2.1. Differential microcalorimetry The microcalorimetrical measurements used to examine the interferences with a waste stabilization process were conducted by means of a differential microcalorimeter of the conduction-isoperibolic type [9]. An ALMEMO 2290-8 data logger was used to register heat effects of the hydration processes in the microcalorimeter, monitoring the change of voltage dU = f(t). The recorded values were processed by a computer program on a computer, obtaining the values of the hydration heat, the relative reaction degree, and the heat-release rate for the given hydration conditions. 2.2.2. Conductivity The conductometrical measurements used to provide the conductivity in the cement pastes were conducted by means of an ISKRA MA 5964 microprocessor conductometer connected to a computer via a RS 232 C digital output. The conductometrical cell electrode was made of stainless steel with a constant C = 0.285 cm-1. 2.2.3. TG analysis Termal analysis were performed on a Pyris 1 TGA at 20 o/min from 50 to 850 oC in 10 ml/min N2 flow. 3. Results and discussion To determine the effect of PbO on OPC hydration, the method of continuous observing of early hydration, microcalorimetry, was applied, which monitors heat released during hydration. Heat released heats the operating cell of a differential microcalorimeter [10], causing a difference of temperatures between the operating and the referent cell, measured as tension difference, dU, by thermocouples. Figure 1 shows the thermovoltage curves for samples of OPC with different additions of PbO. On microcalorimetrical curve for OPC is observed very pronounced second maximum. Increasing the share of PbO maximums assume lower values and the occurrence of the maximum registered in the later hydration times. Figure 1 here Specific conductivity of cement pastes was continuously observed in order to use these curves to determine the conductivity maximums, which indicate the binding time of the cement pastes. Time to appearance of the maximum can be used as a parameter for estimating the share of PbO, which does not delay the binding of cement paste more than the standard allowed time for the beginning and end of the binding. The introduction of PbO into the reaction system leads to slower hydration, but hydration curves have a typical shape with somewhat less intensity of the specific conductivity (Figure 2). Figure 2 here According to the technical specification [11] and standard [12] for OPC, the beginning of binding time should occur after 60 minutes. For the practical application, the end of binding time should happen in time below 200 minutes. It was found that PbO addition to the cement-water system is acceptable up to 0.25 wt. % (Table 3). Increased shares of PbO over 0.25 wt. % significantly delay the beginning of binding time and for the system is not acceptable. Table 3 here Figure 3 shows the thermal curves obtained on heating a hydrated cement samples cured for 28 days. Several losses appear on this curves. Figure 3 here The first between 100 200 oC corresponds to the decomposition of the nearly amorphous hydrates, mainly CSH as well as sulphoaluminate hydrates. The decomposition continues gradually, as evidenced by the slow loss in mass between 200 and 450 oC. A great loss then occurs corresponding to the decomposition of Portlandite (Ca(OH)2). The loss of weight around 700 oC was assumed to represent decomposition of CaCO3. The addition of PbO shifts the peaks to the left and sees a higher mass loss. 4. Conclusion The hydration heat results show that the addition of lead(II) oxide affect the cement hydration kinetics. Kinetic curves show that higher content of lead(II) oxide slow down the hydration processes and the heat values are lower. Addition of lead(II) oxide significantly delays the time appearance of the maximum conductivity. It was found that the acceptable amount of lead (II) oxide in cement system is w = 0,25 wt. %. 5. References [1] R.D. Spence, C. Shi, Stabilization and Solidification of Hazardous, Radioactive, and Mixed Wastes. Boca-Raton: CRC Press, 2005. [2] E. Martens, D. Jacques, T. Van Gerven, L. Wang, D. Mallants, Geochemical modeling of leaching of Ca, Mg, Al, and Pb from cementitious waste forms, Cement Con. Res. 40 (2010) 1298-1305. [3] Q.Y. Chen, M. Tyrer, C.D. Hills, X.M. Yang, P. Carey, Immobilisation of heavy metal in cement-based solidification/stabilization: A review, Waste Manag. 29 (2009) 390-403. [4] M.A.C. Gollmann, M.M. da Silva, A.B. Masuero, J.H. dos Santos, Stabilization and solidification of Pb in cement matrices, J. Hazard. Mater. 179 (2010) 507-514. [5] Z. Giergiczny, A. Krol, Immobilization of heavy metals (Pb, Cu, Cr, Zn, Cd, Mn) in the mineral additions containing concrete composites, J. Hazard. Mater. 160 (2008) 247-255. [6] F.P. Glasser In: R.D. Spencer (Editor), Chemistry and Microstructure of Solidified Waste Forms, Lewis Publishers, Boca Raton, FL, 1993, pp. 140. [7] I.W. Hamilton, N.M. Sammes, Encapsulation of steel foundry dusts in cement mortar, Cem. Concr. Res. 29 (1999) 55 61. [8] C. Tashiro, J. Oba, The effects of Cr2O3, Cu(OH)2, ZnO and PbO on the compressive strength and the hydrates of the hardened C3A paste, Cem. Concr. Res. 9 (1979) 253 258. [9] R. Krstulovi, P. Krolo, T. Feri, Microcalorimetry in cement hydration process, Periodica Polytehnica 33 (1989) 315-321. [10] R. Krstulovi, P. Dabi, A conceptual model of the cement hydration process. Cem. and Concr. Res. 30 (2000) 693-698. [11] Technical specification for CEM I 42,5 R Sv. Juraj [12] EN 196-3, Test Methods for Cement, CEN/TC 51. Figure legends: Figure 1 Thermovoltage curves (dU = f(t)) for the samples with addition of PbO Figure 2 Specific conductivity of cement paste containing PbO Figure 3 Thermal analysis of a hydrated cement sample with addition of PbO, cured for 28 days Table 1 Chemical composition of OPC _________________________________________ Compositions (%) OPC ______________________________________________ SiO2 22.85 Al2O3 4.81 Fe2O3 2.79 CaO 65.23 MgO 1.61 K2O 1.89 Na2O 0.18 Loss of ignition 0.04 _______________________________________________ Table 2 Physical and mechanical properties of OPC Physical property ValueSpecific surface according to Blaine (cm2 g1) 3300 Standard consistency (%) 26 &8JPV  :    0 2 6 j    . / 1 = x y  һһһݛ}}hOmH sH hO0JmH sH hzMhihOH*hOjhOhOUjhOhOUhOhO0JjhOhOUjhOhOUhOhO5 hOhOh& h)_5 h\D5 h~51 : 6 T j 1 = h fgw $da$gdO $da$gdOdgdO$a$gd~fppp '(\]mnrs|}%&*+<=UVoq}~efgwҾhOh~5h~hOh$hOhO5 hOhOhRhOmH sH hO0JmH sH hO0JmH sH hOmH sH Fw2:[tvUv~ $3745J}~9Xcklՙ{hjmH sH hj0JmH sH hehjhgkhhmH sH hhE]hE]H*hE]hE]h)?)E)F)N)O)U)V)d)e)n)μƴμhmH sH h0JmH sH hn)}0JmH sH hLfmH sH hLf0JmH sH h"mH sH h"0JmH sH h"\mH sH hUf\mH sH hThUf\mH sH hUf\mH sH ,F,G,M,i,j,,-@-A-C------------. . ..... .!.%.&.../.9.:.;.ȼȴvhUZ80JmH sH h]E=0JmH sH hk70JmH sH hlmH sH hk7hk7H*mH sH hlhk7H*mH sH hk7mH sH h0h0H*mH sH h0mH sH h*Ph*Ph*PH*mH sH hqwmH sH h*PmH sH h]E=mH sH hfmH sH (;.I.-/./J/W/X/^/_/g/h/u/v////////////////////////000z0000>1?1йЮ{sh 4mH sH hfHmH sH  hKhhfHhhmH sH h 4h5mH sH hmH sH hh7 mH sH h7 0JmH sH h7 hUZ80JmH sH h7 mH sH h7 0JmH sH h7 h7 mH sH h7 hhUZ80J5mH sH ,I../////0?112F33V4567 8S8T8 $da$gd$d7$8$H$a$gdxr$d7$8$H$a$gd$d7$8$H$a$gdPQ $da$gd 4 $da$gd$ & Fda$gd7 ?1C11111222E3F3I3J3r333333333#4$4V4Z44444444444445 5666666(6*6b6d66ʷʷЪ h1'hhhhH* hhhmH sH hPQ hPQhPQ hSS^0JhPQhPQ0JhPQhPQ0J] hPQ0JhPQmH sH hSS^mH sH hZmH sH hTomH sH hy*FmH sH h;mH sH 266666666~77777778 8#8$8O8R8d8r8s8|8}8888888999ӾӶyqiq]hhf5mH sH hfmH sH hcmH sH hc\mH sH hhc5hc h5hh"J5h"JhKmH sH hPQhxrh;mH sH h;mH sH hxr hxrhxrCJOJQJ^JaJ hxrhxrhxrhxrmH sH h h1'h hhh h6"T8U8V8W8X8Y8Z8[8\8]8^8_8`8a8b8c8d8t889_9`9a9b9c9d9e9f9g9 $da$gd9 9_9r9s9z9~99999999:::::%:&:':(:-:4:5:6:7:<:]:^:k:l::::::;;[;;;ƿѦƮƞƞƞƞƞƞƞ摉xpk hH*hr9h5hu h5h h5h'[h5hmH sH  h\#H*hMh\#H*hu h\#5 h|h\#h\#OJQJ^J hu h\#h\# h; h\# h\#5h'[h\#5h&4mH sH h\#mH sH hfmH sH h&45mH sH *g9h9i9j9k9l9m9n9o9p9q9r9s9999:#:2:A:O:\:i:w:$d`a$gd{A $7$8$H$a$gd{A$d7$8$H$a$gd{A $da$gdw::::::::::::::::;;[;$d$Ifa$gd&4 $da$gd $da$gd $da$gd\# $da$gd{A$d`a$gd{A[;\;;;Wlll+mmm nfn$d$Ifa$gd&4kkd$$IfTlP^ t0644 la^T ;;;;lllgnsnxnzn{nnnnnnnnnnnoooooo%o&o0o1oDoEoFoNooooooooooɾɶqjhmUmHnHuhmmH sH h\mH sH jh1h1Uhh5jb h1h1UhCJaJhmh\hfh&4mH sH h&4mH sH hh&45mH sH h&45mH sH hmH sH h%UhesQhH*h,Setting time start (min) 85 Setting time end (min) 150 Average flexural strength (MPa) after 3 days 6.26 after 28 days 8.44 Average compressive strength (MPa) after 3 days 33.5 after 28 days 50.7 Table 3 Time to maximum appearance for various addition of PbO Addition of PbOTime to maximum appearancewt. %min0,001050,051150,101350,252050,505600,7510601,001780  Figure 1 Thermovoltage curves (dU = f(t)) for the samples with addition of PbO  Figure 2 Specific conductivity of cement paste containing PbO  Figure 3 Thermal analysis of a hydrated cement sample with addition of PbO, cured for 28 days     PAGE  PAGE 6 CEM I 0.2 PbO 0.3 PbO 0.4 PbO 0.5 PbO 0.6 PbO 0.7 PbO fngnhninjnknlnmnnnonpnqnrnsnn} $da$gd{A $da$gdkkd$$IfTlP^ t0644 la^TnnnnnnbkdE$$IfTl;0r'|'(644 labpT $$Ifa$gd&4nnnnnn/bkd$$IfTl;0r'|'(644 labpT $$Ifa$gd&4bkd$$IfTlJ0r'|'(644 labpTnnnooo/bkde$$IfTl;0r'|'(644 labpTbkd$$IfTl;0r'|'(644 labpT $$Ifa$gd&4o ooooobkd4$$IfTl;0r'|'(644 labpT $$Ifa$gd&4oo o%o&o+o/bkd$$IfTl;0r'|'(644 labpT $$Ifa$gd&4bkd$$IfTl;0r'|'(644 labpT+o0o1o2o3o4o5o6o7o8o9o:o;oo?o@oAoBoCoDoFoooooooooooooooooooo $da$gd $da$gdoooooooooooopppppppp`pepfphpipkp $da$gd{Adgddgd&4 $da$gdooppppepfpgpipjplpmpoppprpspypzp{p}p~ppppppppppphmhfHhK0JmHnHu h0Jjh0JUhjhUhh{AmH sH h{A5mH sH hh{A5mH sH h{AmH sH hmH sH hmmH sH kplpnpopqprp{p|p}pppppppppppppppppppgdmh]hgd &`#$gdfHpppdgd,1h. 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