Vol.30 No.2 LIU Fengli et al: Basic Properties of Concrete Incorporating Recycled Cer... 352 DOI 10.1007/s11595-015-1152-3 Basic Properties of Concrete Incorporating Recycled Ceramic Aggregate and Ultra-fine Sand LIU Fengli1,3, LIU Junhua2, MA Baoguo3*, HUANG Jian3, LI Hainan3 (1. Institute of Material and Structure, Henan University, Kaifeng 475004, China; 2. School of Civil Engineering and Architecture, Kaifeng University, Kaifeng 475004, China; 3. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China) Abstract: Recycled ceramic mixed sand (RCMS) was obtained by partially replacing ultra-fine sand with recycled ceramic coarse sand (RCCS). The effects of RCCS replacement rate on the apparent density, workability, compressive strength and splitting tensile strength of recycled ceramic concrete (RCC) were investigated. In addition, the relationship between the water-cement ratio and compressive strength of RCC was also studied. The experimental results indicate that the reusing of recycled ceramic aggregate can improve the cohesiveness and water retentiveness of fresh concrete and benefit the mechanical properties development. When the RCCS replacement rate is not less than 40%, the mechanical properties of RCC are superior to those of the reference concrete. Moreover, when recycled ceramic medium sand was completely used as fine aggregate, the maximum increase in both compressive strength and splitting tensile strength were obtained, comparing with those of reference concrete, the increment ratio was 19.85% and 32.73%, respectively. The microscopic analysis shows that the using of recycled ceramic aggregate can meliorate distinctly the structure of the interfacial transition zone (ITZ) and increase the compaction degree of cement paste. Furthermore, an expression of the compressive strength of RCC and the cement-water ratio is regressed and gains a good linear relativity. It is an effective way to recycle waste ceramic, and the consumption of recycled ceramic aggregate could reach from 26.9% to 47.6% of the total weight of aggregate in producing concrete. Key words: recycled ceramic coarse sand (RCCS); ultra-fine sand; recycled ceramic concrete (RCC); property; regression analysis; sustainability 1 Introduction China has been the world's biggest ceramic production nation in the past 13 years. The output of waste ceramic reached more than ten million tons every year[1]. Due to its poor biodegradability, waste ceramic has caused serious destruction to environment, especially in ceramic producing areas. Recycling waste ceramic can bring us great social, economic and environmental benefits. Construction consumes enormous amounts of building materials. The ©Wuhan University of Technology and SpringerVerlag Berlin Heidelberg 2015 (Received: May 22, 2014; Acceted: Aug. 5, 2014) LIU Fengli (刘凤利): E-mail: lfl@henu.edu.cn *Corresponding author: MA Baoguo (马保国): Prof.; Ph D; E-mail: mbgjob@163.com Funded by the National Natural Science Foundation of China (No.50902107) and the Fundamental Research Funds for the Central Universities (No.2013-YB-25) application of waste ceramic in building materials is of potential research value. Many scholars, at home or abroad, make a lot of experimental research on it, and have made certain theoretical achievement. The results of relevant research can be classified as follows: Firstly, it was used as mineral admixture with pozzolanic effect for concrete or mortar. Silva et al[2] drew conclusion that a good workability of fresh mortar and high compaction degree of hardened cement pastes could be achieved by partially replacing cement with polished ceramic powder. Cheng et al[3] hold that it could lower the carbonation resistance and improve the sulphate corrosion resistance of concrete when ceramic polishing powder was used as a supplementary cementing material in concrete. Secondly, waste ceramic was crushed into fine aggregate which was partly or completely used to replace natural sand in mortar or concrete manufacture. Jimenez et al[4] and Higashiyama et al [5] provided some examples of such studies. And some positive results were obtained. Thirdly, it Journal of Wuhan University of Technology-Mater. Sci. Ed. www.jwutms.net Apr.2015 was used as recycled coarse aggregate by partial or complete substituting for ordinary coarse aggregate. Studies [6-11] on the basic mechanical properties and microstructure of recycled ceramic concrete (RCC) concluded that it was feasible to prepare concrete or mortar with recycled ceramic aggregate. Still, there is a big gap on behavior of concrete that incorporates ultrafine sand and recycled ceramic aggregate as both fine and coarse aggregate. Because of the thin slice shape (thickness often between 3 mm and 10 mm) and glaze surface of waste ceramic products, the particle size of recycled ceramic aggregate should not be too large. However, it often presents the following problems: Firstly, high schistose grain content, which is detrimental to the workability and mechanical properties of concrete. Secondly, high proportions of glaze surface, which would greatly weaken the bond strength between aggregate and hardened cement paste. Namely, particle shape and surface morphology of recycled ceramic aggregate are critical to the properties of RCC. Meanwhile, in the view of energy consumption on waste ceramic fragmentation, it was recommended that waste ceramic is preferably used as coarse sand so as to save energy, and it is also conducive to incorporating recycled ceramic aggregate and ultra-fine sand and making full use of the two resources. When waste ceramic is used to prepare recycled coarse aggregate, it’s good to make particles under 10mm which is often the maximum thickness of a ceramic tile. Wan et al[12] replaced natural coarse aggregate with recycled ceramic coarse aggregate (fraction size between 5 mm and 20 mm) in concrete production, and concluded that the cubic compression strength, axial compressive strength and splitting tensile strength are lower than those of ordinary concrete. Ding et al[13] carried out the comparative experiments between conventional concrete and RCC in which gravel was partially (0, 15%, 30%, 45%, 60%, and 100%) replaced by recycled ceramic coarse aggregate (fraction size between 5 mm and 25 mm), and reached similar conclusion that it will weaken the strength of concrete when the substitution ratio of recycled ceramic coarse aggregate increased. However, the recycled ceramic aggregate used in the two experiments described above had good gradation and higher strength than those of natural coarse aggregate. But why did RCC present lower strength? It is perhaps just owing to that the particle size of recycled ceramic coarse aggregate was too large. And the particle shape (flat instead of 353 spherical or cubic) and surface morphology (smooth instead of rough) of recycled ceramic coarse aggregate play negative role on the mechanical properties of concrete. Instead, Medina et al [7-10] proved that the microstructure present in the interfacial transition zone (ITZ) of the recycled aggregate-paste was more compact and stable than that of the natural aggregatepaste, and reached similar results in mechanical behavior comparison between RCC and ordinary concrete by using recycled ceramic coarse aggregate with particle size of 4/12.5 mm. Halicka et al[11] also obtained higher compressive strength and tensile strength of RCC than those of the reference concrete. Combining the current situation that China is rich in ultra-fine sand and gross underuse, this article studied the incorporation of recycled ceramic aggregate and ultra-fine sand on concrete production. The objective pursued was to analyze the effect of the incorporation of recycled ceramic aggregate and ultra-fine sand on the properties of concrete. And experiments were carried out to research the effects of the variation of both replacement rate of recycled ceramic coarse sand (RCCS) and cement-water ratio on the properties of RCC. 2 Experimental 2.1 Materials The materials used to fabricate concrete were cement, nature medium sand, recycled ceramic mixed sand (RCMS: the mixture of ultra-fine sand and RCCS), recycled ceramic medium sand and crushed stone. Fig.1 shows the shape and morphology of RCCS and ultrafine sand. PO 42.5 cement was used as the cementitious material. The physical and mechanical properties of cement are listed in Table 1. Ultra-fine sand came from the local Yellow river. The particle size distribution of ultra-fine sand is shown in Fig.2. The waste ceramic used was floor tiles and wall tiles obtained locally from housing demolition. Waste ceramic were crushed with a jaw crusher and sieved into particles under 9.5 mm. The particle size of the crushed ceramic was sorted into three classes according to their particle size distributions: RCCS, recycled ceramic medium sand and recycled ceramic coarse aggregate, respectively. The physical properties of the coarse and fine aggregate are presented in Table 2. As shown in Table 2, recycled ceramic aggregate has the following characteristics: angular, rough surface, high water absorption and low density when compared to natural sand. The sieving results of 354 Vol.30 No.2 LIU Fengli et al: Basic Properties of Concrete Incorporating Recycled Cer... fine aggregate are also shown in Table 3. Additionally, the water used was tap water. Fig.1 Pictures of (a) RCCS and (b) ultra-fine sand Fig.2 Particle size distrbution of ultra-fine sand RCCS was mixed with ultra-fine sand with different proportions to prepare recycled ceramic mixed sand (RCMS). Recycled ceramic coarse aggregate (4.75/9.5 mm) was used to completely replace the same size particles of crushed stone. The most important difference between the natural aggregate and the recycled ceramic aggregate was their physical shape and surface texture. Recycled ceramic aggregate was irregularly shaped and had rough surface, while the shape of the natural aggregate used could be considered as more rounded and smooth than that of recycled ceramic aggregate. 2.2 Methods The concrete samples were sized at 150 mm×150 mm×150 mm. The slump and apparent density of fresh concrete were tested according to GB/T 500802002 “Standard for Test Method of Performance on Ordinary Fresh Concrete” [14]. The compressive strength and splitting tensile strength of concrete were tested according to GB/T 50081-2002 “Standard for Test Method of Mechanical Properties on Ordinary Concrete”[15]. The morphology and microstructure of the cement paste and the interfacial transition zone (ITZ) between the aggregate and cement matrix were investigated with a Japanese D/Max-RB scanning electron microscope (SEM). In addition, some samples were cut, polished, and then analyzed by SEM-EDS. 3 Results and discussion 3.1 Effect of RCCS replacement rate on properties of concrete The replacement rate of RCCS has important Journal of Wuhan University of Technology-Mater. Sci. Ed. www.jwutms.net Apr.2015 effect on the properties of RCMS, it determents the gradation and the average particle size of RCMS, and also has impact on its particle shape and surface morphology. Therefore, experimental studies on some basic properties of concrete with RCMS as fine aggregate were carried out. 3.1.1 Mix proportion A total of six concrete mixes were produced and the mix proportions are shown in Table 4. The reference concrete (sample number was NF as noted in Table 4) was prepared with natural medium sand as the fine aggregate and crushed stone as the coarse aggregate. Four recycled concrete mixes were prepared using RCMS (replacing ultra-fine sand with RCCS at the levels of 20%, 40%, 60%, and 80%, respectively). The sieving results of the above RCMS are listed in Table 5. In addition, one concrete mix (sample number was RF as noted in Table 4) using recycled ceramic medium sand as the fine aggregate was also prepared. In view that recycled ceramic aggregate has the feature of high water absorption, apart from the free water, the absorbed water, based on the different water absorption values between recycled ceramic aggregate and the ultra-fine sand, which would absorbed completely by recycled ceramic aggregate was added to the mixing water. 3.1.2 Apparent density of fresh concrete Experimental results of the apparent density of fresh concrete are presented in Fig.3. Overall, incorporating RCCS and ultra-fine sand as fine aggregate decreased the apparent density of RCC when compared to the reference concrete (NF). And it is evident that the apparent density of RCC decreased gradually with the increase of RCCS replacement 355 rate. The decreasing ratio of apparent density by incorporating 20%, 40%, 60%, and 80% of RCCS was 0.42%, 1.26%, 2.10%, and 2.94%, respectively. And the apparent density of concrete with recycled ceramic medium sand as fine aggregate (RF) was 3.36% lower than that of the reference concrete (NF). With the increase of replacement rate of RCCS, the apparent density of RCC gradually decreased. The key reason for this could be that recycled ceramic aggregate has smaller apparent density and its rough surface can lead to large air-entraining and so on. After concrete was cut and polished, a typical cross section of aggregate was exposed. The SEM images of RCCS and ultra-fine sand are presented in Fig.4. As shown in Fig.4, RCCS is more porous than ultra-fine sand. There are a lot of little pores distributed in the cross section of RCCS, whereas that of the ultra-fine sand is compact. And the high porosity of RCCS is the main reason causing a reduction in its apparent density. The decrease in apparent density of RCC is advantageous 356 Vol.30 No.2 LIU Fengli et al: Basic Properties of Concrete Incorporating Recycled Cer... to reduce the self-weight of buildings and develop the long-span structures. concrete (NF). The increasing ratio of compressive strength by incorporating 20%, 40%, 60% and 80% of RCCS was 8.68%, 6.95%, 1.99% and 8.44%, respectively. The maximum improvement (19.85%) occurred when completely using recycled ceramic medium sand as the fine aggregate. Fig.4 SEM images of (a) fine aggregate in concrete and (b) cross section of RCCS 3.1.3 Workability Experimental results of the slump of fresh concrete are presented in Table 6. As seen in Table 6, similar concrete slump values (50/60 mm) were obtained. And based on the observation of concrete mixture, it was found that RCC has the better cohesiveness and water retentiveness than those of the reference concrete (NF). When the replacement rate of RCCS was increased (from 20% to 80%), more absorbed water in the mixing water was required to maintain the similar workability of fresh concrete. Because recycled ceramic aggregate has the features as follows: angular, rough surface, high porosity and high water absorption, under the condition of the same mixing proportion, recycled concrete with recycled ceramic aggregate would exhibit a lower fluidity. The present experimental results indicate that through adding absorbed water, RCC can reach similar fluidity with the reference concrete. And adding absorbed water in the traditional mixing proportion of concrete proved to be an effective way to solve the decrease in slump of fresh concrete. The main reason of improvement in cohesiveness and water retentiveness with the inclusion of recycled ceramic aggregate may be attributed to the increase in friction between aggregate and cement paste due to their angular shape and rough surface. 3.1.4 Compressive strength The experimental results of the compressive strength of concrete are presented in Fig.5. The results indicate that the compressive strength of RCC did not change significantly with increasing RCCS content, when absorbed water was added in the mixing water. However, it was higher than that of the reference The reason why compressive strength of RCC was higher than that of the reference concrete (NF) may attribute to the following factors: firstly, RCCS has irregular shape and rough surface, which could enable good meshing effect between aggregate and hardened cement paste. Secondly, ceramic micro powder generated during the fragmentation processes has pozzolanic activity which could act as supplementary cementing material in RCC. Thirdly, the effect of internal curing, due to high porosity and high water absorption of RCCS, provided guarantees for the hydration of cement and concrete strength development in the later age. Fourthly, it is generally known that the performance of the interfacial transition zone (ITZ) and the strength of hardened cement stone are weak areas which often cause the damage of concrete. So the major reason for higher compressive strength of RCC may be that the properties of RCCS, such as high water absorption, having ceramic micro powder on surface, improved the performance of the interfacial transition zone (ITZ) between aggregate and hardened cement stone. Meanwhile, the high water absorption of RCCS can reduce the effective water-cement ratio of cement paste, thereby giving higher strength of hardened cement stone. 3.1.5 Splitting tensile strength The experimental results of the splitting tensile strength of concrete are presented in Fig.6. Similar to the results of compressive strength, the splitting tensile strength of RCC did not change significantly with increasing RCCS content, when absorbed water was added in the mixing water. The increasing ratio of the splitting tensile strength by incorporating 40%, 60%, Journal of Wuhan University of Technology-Mater. Sci. Ed. www.jwutms.net Apr.2015 and 80% of RCCS was 16.55%, 2.52%, and 30.94%, respectively. When ultra-fine sand was replaced by RCCS with 20%, the splitting tensile strength of RCC was decreased by 12.6%. Similarly, the maximum increment (32.73%) occurred when recycled ceramic medium sand was used completely as the fine aggregate. The above mentioned results related to the variation of RCMS properties, such as gradation, average particle size, average water absorption, the shape and surface roughness of aggregate etc., when the percentage of RCCS is different. The positive effect on the splitting tensile strength is probably due mainly to the angular shape and rough surface of RCCS which increased the meshing force between the aggregate and cement matrix. The variation law of splitting tensile strength was not obvious. Nevertheless, when the RCCS replacement rate is equal to or higher than 40%, the splitting tensile strength is higher than that of the reference concrete. And surely there were ways in which RCC meeting the required splitting tensile strength could be obtained by adjusting the replacement rate of RCCS. 3.1.6 SEM analysis 357 are shown in Fig.7. SEM images of the interfacial transition zone (ITZ) in RCC at 150×, 2400×, and 5000× respectively are presented in Fig.8. Fig.8 SEM images of the interfacial transition zone (ITZ) in RCC: (a) 150×; (b) 2400×;(c) 5000× Fig.7 and Fig.8 show that the RCC has a denser paste in the range of the interfacial transition zone (ITZ) than that of the reference concrete (NF). It can be seen from Fig.7 (a) that there are a large amount of large dendrite crystals and plenty of micro-pores in the interfacial transition zone (ITZ) between natural medium sand and cement matrix, as indicated by white circles. Instead, the properties of the interfacial transition zone (ITZ) between RCCS and cement matrix were homogenized with the bulk. Those results prove that the using of recycled ceramic aggregate can meliorate distinctly the structure of the interfacial transition zone (ITZ) of the concrete, thus the strength of concrete is improved. The morphology of the hydration products in cement paste of different concrete is presented in Fig.9. Fig.7 SEM images of the interfacial transition zone (ITZ): (a) between natural medium sand and cement matrix; (b) between RCCS and cement matrix In order to find a plausible reason for the results of the above described tests, some scanning electron microscope (SEM) observations of concrete samples were performed. SEM images of the interfacial transition zone (ITZ) in concrete with different fine aggregate obtained with a magnification of 5000× Fig.9 SEM images of the hydration products: (a) concrete with natural medium sand; (b) concrete with RCMS Because recycled ceramic aggregate has features of high porosity and high water absorption, the 358 Vol.30 No.2 LIU Fengli et al: Basic Properties of Concrete Incorporating Recycled Cer... effective water-cement ratio (w/c) was reduced at some levels. Besides, micro powder of ceramic generated during the fragmentation processes can perform pozzolanic reaction which could increase the number of hydrated products and fill the micro-pores and microcracks in the cement paste. Those factors are conducive to improving the compaction degree of the cement matrix. As shown in Fig.8, the cement paste of RCC has a more compact matrix and significantly smaller macro-pores than that of the reference concrete (NF). And that is one of the reasons that RCC proved to have higher strength than the reference concrete. 3.1.7 SEM-EDS analysis The microstructure and element distribution of the interfacial transition zone (ITZ) in different concrete were investigated by using both scanning electron microscope (SEM) and X-ray energy dispersive analysis (EDS). Fig.10 shows the SEM-EDS images of the interfacial transition zone (ITZ) in the reference concrete (NF). And the SEM-EDS images of the interfacial transition zone (ITZ) in the RCC are indicated in Fig.11. Fig.10 SEM image (a) and EDS spectra (b) of the ITZ of the reference concrete (NF) As shown in Fig.10 (a) and Fig.11 (a), there is a micro-crack in the interfacial transition zone (ITZ) between natural sand and cement matrix in the reference concrete (NF), whereas the interfacial transition zone (ITZ) between RCCS and cement matrix in RCC is compact. Two major hydrated products of Portland cement are hydrated calcium silicate (C-S-H) Fig.11 SEM image (a) and EDS spectra (b) of the RCC gel and calcium hydroxide (CH), occupying about 70% and 20% of the total hydrated products respectively. It is obvious that the more CH, the higher the mole ratio of Ca to Si. Comparing Fig.10 (b) and Fig.11 (b), it can be seen that the mole ratio of Ca to Si at the interfacial transition zone (ITZ) of the reference concrete is higher than that of the interfacial transition zone (ITZ) in RCC. Namely, the interfacial transition zone (ITZ) in RCC has lower CH content and more C-S-H gel. And it was good for decreasing the porosity and enhancing the bonding force of the interfacial transition zone (ITZ). 3.2 Effect of water-cement ratio on compressive strength of concrete The properties of recycled ceramic aggregate are different from natural aggregate which is usually used in ordinary concrete, hence Bolomey formula obtained in terms of ordinary concrete no longer applies to RCC. In the present paper, the relationship between compressive strength of RCC and cement-water ratio was investigated, and regression coefficients which are quite different from that of ordinary concrete was obtained. 3.2.1 Mixing proportion Using recycled ceramic medium sand as fine aggregate, and recycled ceramic coarse aggregate (particle size of 4.75/9.5 mm) incorporating with crushed stone (particle size of 9.5/31.5 mm) as coarse aggregate, seven concrete mixes were prepared for this Journal of Wuhan University of Technology-Mater. Sci. Ed. www.jwutms.net Apr.2015 study as indicated in Table 7 from sample RC-0.44 to RC-0.74, in which the water-cement ratio was from 0.44 to 0.74 with an increment of 0.05. 359 the regressive coefficient. It could provide reference for the mixing proportion design of RCC. 4 Conclusions 3.2.2 Results and regression analysis Results of the 28-day compressive strength of RCC are presented in Table 8. Then regression analysis was used and the results are presented in Fig.12. The relationship between the 28-day compressive strength of RCC and cement-water ratio is worked out with the help of regression analysis, and expressed as follows: (1) or: (2) where, fcu,28 is the compressive strength of RCC at 28 d, MPa; c/w is the cement-water ratio; fce is the measured strength of cement at 28 d, MPa, and fce equals 50.7 MPa in this experiment. The regressive coefficients obtained by regression analysis are as follows: A=0.278, B=2.058. And the result reveals that the compressive strength of RCC also has good linear relationship with cement-water ratio, similar to that of ordinary concrete. The difference is a) The particle size of recycled ceramic aggregate should not be too large. The thickness of waste ceramic products is the critical factor determining the particle size. It is feasible to reuse recycled ceramic aggregate (under 9.5 mm) in partial replacement of natural aggregate in the manufacture of concrete. It is an easy and effective way to use RCMS (incorporating RCCS and ultra-fine sand with proper proportions) as a kind of sustainable green aggregate. b) The apparent density of RCC is lower than that of ordinary concrete. It is helpful to reduce the selfweight of constructions. Under similar workability condition, when the RCCS replacement rate is no higher than 20%, the splitting tensile strength of RCC is poor because the ultra-fine sand has high mud content and for other reasons. And when the RCCS replacement rate is no less than 40%, the compressive strength and splitting tensile strength are higher than those of the reference concrete. When recycled ceramic medium sand was completely used as fine aggregate, the maximum increase in both compressive strength and splitting tensile strength was obtained, comparing with those of the reference concrete, the increment ratio is 19.85% and 32.73%, respectively. c) RCC has more compact and homogeneous interfacial transition zone (ITZ) than that of the reference concrete (NF). In addition, the interfacial transition zone (ITZ) in RCC has low CH content and more C-S-H gel. The using of recycled ceramic aggregate can meliorate distinctly the structure of the interfacial transition zone (ITZ) of the concrete. Vol.30 No.2 LIU Fengli et al: Basic Properties of Concrete Incorporating Recycled Cer... 360 Moreover, the cement paste of RCC has a more compact matrix and significantly smaller macro-pores than that of the reference concrete (NF). And those are the key reasons that RCC proved to have higher strength than the reference concrete. d) The compressive strength of RCC also has good linear relationship with cement-water ratio, similar to that of ordinary concrete, but they have different regressive coefficients in regression formula. An expression of the compressive strength of RCC and the cement-water ratio is regressed and gains a good linear relativity. It provides reference for the mixing proportion design of RCC. e) The consumption of recycled ceramic aggregate could reach from 26.9% to 47.6% of the total weight of the fine and coarse aggregates in producing concrete, and this method of recycling waste ceramic is energysaving and environment friendly. [5] Higashiyama H, Kiyoshi Yamauchi, et al. A Visual Investigation on Chloride Ingress into Ceramic Waste Aggregate Mortars Having Different Water to Cement Ratios[J]. Construction and Building Materials, 2013, 40: 1 021-1 028 [6] Guerra I, Vivar I, Llamas B, et al. 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