1. Introduction
The construction industry faces significant challenges in maintaining sustainability within today’s environmental context. This is primarily due to the cement industry grappling with the contradicting factors of meeting the substantial demand for raw clinker production and minimizing the industry’s CO
2 emissions [
1].
The rapid urbanization and post-war demolition in Europe have resulted in significant amounts of construction and demolition waste (CDW), attracting academic attention due to its potential for secondary use [
2]. The movements mentioned above contribute significantly to total waste generation. In the European Union (EU), CDW accounts for over 36% of all waste produced [
3]. The EU has established ambitious objectives for upcycling CDW in response to this challenge. Leveraging CDW as a secondary raw material offers dual environmental advantages, such as decreasing the demand for mineral natural resources and diminishing the waste sent to landfills.
Fine recycled aggregate (fRA) utilization practices commonly entail low-value applications like backfilling, relegating its potential to landfills, or indefinite stockpiling at CDW facilities. This highlights the importance of setting specific goals for fRA under the European Union’s Circular Economy Action Plan [
3]. To advance the market reach of fRA, a shift towards more valuable applications is necessary. This can be facilitated through innovative methods like additive concrete manufacturing, which can drive a paradigm shift. This strategic reorientation aligns with circularity principles and emphasizes the importance of using technological advancements to promote sustainable resource utilization in the construction industry.
This paper concerns the applicability of fine recycled aggregates (fRA) produced from 3D printed concrete waste (in practical terms, ultra-high-performance concrete (UHPC) waste). Research has demonstrated that recycled aggregates produced from ultra-high-performance concrete (UHPC) tend to be better suited for use in concrete than recycled aggregates produced from lower-quality waste [
4]. This is partly due to the higher cement content of UHPC, often around 1100 kg/m
3, which is more than three times that of the cement content of conventional concrete [
5]. However, using recycled aggregates in concrete can adversely affect its fresh and hardened properties [
6].
With the advent of concrete 3D printing, specific criteria such as extrudability, buildability, and setting time must be met through the mixed formulation design of 3D printed concrete (3DPC). As a result, a substantial quantity of binder, primarily cement, is needed, with a quantity exceeding 700 kg/m
3, which is more than two times that of conventional concrete [
7,
8]. Pacheco et al. [
9] conducted a literature survey that concluded that most 3DPC mixes contain binder contents exceeding 500 kg/m
3. In addition, aggregate sizes greater than 4 mm are typically excluded from 3DPC mix designs, with a maximum aggregate size of 2 mm being recommended. This requirement is due to pump limitations and the need for narrow cross-section layers, resulting in a considerable demand for river sand in 3D printing. This poses a severe risk to natural resources, due to the high ratio of fine aggregates. In conjunction with the increasing real-world developments in concrete 3D printing, the above facts have demonstrated that recycled aggregates obtained from 3DPC waste have immense potential to serve as a secondary material source after recycling.
Currently, there is a shortage of knowledge regarding the use of fRA in 3D printing. Employing recycled aggregates as a substitute for natural aggregates is considered a viable solution to tackle the issue of CDW accumulation and minimize the extraction of natural resources [
10,
11]. For instance, Ding et al. [
12] studied the impact of incorporating fine recycled aggregates on the mechanical performance of 3D printed concrete. Their results indicated a slight decrease in the compressive and flexural strengths of the 3D printed samples that contained fine recycled aggregates compared to those that used natural sand. Moreover, the compressive, tensile splitting, and flexural strengths of the recycled sand 3D printed concrete were significantly anisotropic. As previously stated, while there may be some slight decay in performance, research has shown that 3D printed concrete made using recycled aggregates still performs satisfactorily [
12,
13,
14,
15]. Additionally, several proposed methods have been made for improving the properties of these aggregates, including carbonation modification, which has been proven effective at enhancing the recycled fine aggregates and aiding in carbon dioxide sequestration [
11].
This research explores the potential use of recycled fine aggregates from 3DPC waste in additive manufacturing as a substitute for cement. While one paper [
16] has reported incorporating recycled fine powder waste as a cement substitute, it required grinding the CDW down to less than 75 microns. To the best of our knowledge, no study has yet examined the feasibility of using fRA derived from recycled 3DPC waste as a cement substitute in 3DCP without adding extra mixing water and applying extreme energy-consuming grinding processes.
Although some of the characteristics of fRA, such as high water absorption and rough texture, are undesirable for conventional concrete, if a proper mix design is carried out, they are advantages for a 3D printed concrete mix design, since they may be used to tailor the rheological properties of a 3D printed mix (ensure proper buildability and extrudability), allowing decreases in cement content. To date, there is limited knowledge on the application of fRA for 3D printing applications; however, some research groups have confirmed their satisfactory performance in 3D printed concrete [
12,
14,
17].
Based on the abovementioned literature and scarce information on the design of 3DPC with fRA, a preliminary study was conducted to optimize the mix design by including fRA produced from the recycling of 3DPC. The following hypotheses were studied in this paper:
The rougher texture and the much higher water absorption of an fRA in comparison to natural fine aggregates imply that an extrudable mix increases its strength earlier, increasing the buildability as time passes (but decreasing extrudability);
If a proper balance is reached, optimizing the mixture design to achieve lower cement content by introducing fRA in the mix is possible.
These hypotheses were the basis for an experimental program in which the following occurred:
Starting with a reference mix, mortars for 3DPC were developed by replacing the cement with fRA at different replacement ratios;
The fresh-state hardened mechanical properties and the extrudability and buildability of the 3DPC mixes tested were studied;
To better understand the influence of the fRA on the properties of 3DPC, the superplasticizer dosage remained fixed for all mixes;
The 3D printing process of the testing columns was performed in the same printing conditions (fixed printing parameters, including speed and methodology);
A comparative life cycle assessment (LCA) was used to quantify the environmental and economic benefits of replacing cement with fRA.
As a first approximation, it was assumed that no changes to the water content of the mix were needed. This is because cement replacement (smaller particle size and higher surface area) is compensated by rough surface of fRA, which has high water absorption rates. This hypothesis was compared with a workability window that was defined based on slump flow testing.
The assumptions and experimental design are part of a comprehensive research program to find alternatives for using fRA in 3DPC. The present study aims to simplify a mix design procedure that maximizes the environmental benefits of this replacement (since cement is replaced with fRA without additional changes to the mix design) at a technical cost (presumed loss of open time, workability, and extrudability). Other experiments are ongoing and aim to maximize the fresh- and hardened-state technical performance.
4. Discussion
The paper addresses a critical issue related to the development of sustainable 3D concrete printing technology in terms of the reduction in cement content in 3D printed mixes. This study evaluated the potential strategy of substituting cement with fine recycled aggregate produced from recycled 3D printed structures.
The slump flow of the designed mixes after 15 min of water contact aligns with findings from other studies in the field (i.e., [
32,
33,
34]). However, after 30 min of water contact, the mean diameter of the flow for mixes R40 and R50 falls below the printability region, while, for R30, the printability window is shortened. This phenomenon is attributed to the high water absorption rate of the used aggregate; nonetheless, this situation hinders the possibility of printing. Therefore, based only on the slump flow, it can be concluded that replacing cement with fine recycled aggregates (fRA) without modifying the mixture design with chemical admixtures is reasonable for a maximum replacement rate of 20% by volume (mixes R10 and R20).
The evaluation of the green strength and buildability during the printing process indicates that the results are sufficient for the printing process. Firstly, it should be noted that the green strength obtained for materials modified with the fine recycled aggregate (fRA) ranges between 5.27 kPa and 11.09 kPa after 30 min and between 6.26 kPa and 14.73 kPa for specimens tested for 60 min. These values are in line with those presented in other studies [
13,
15,
30,
32,
50]. Chosen research teams that focused on ordinary mixes without recycled aggregate incorporation obtained the following results after 30 min: Casagrande et al. [
32] reported values of between 4.30 kPa and 26.04 kPa, Wolfs et al. [
50] reported about 10.5 kPa, Panda et al. [
51] reported about 10.65 kPa, and Skibicki et al. [
30] reported about 9.02 kPa. The analyses of these studies prove that the obtained results are within the boundaries that demonstrate printing potential. Other studies dedicated to the incorporation of recycled aggregates present inconclusive results. For example, Ding et al. [
15] indicate an increase in green strength after incorporating recycled sand, from 10.68 to 12.23 kPa, while Skibicki et al. [
13] prove that the addition of recycled aggregate leads to a decrease in green properties (from about 14 kPa to 3.8 kPa). Based on the presented examples, (i) in both studies, the recycled aggregate was used as a substitution for a natural aggregate, while, in the presented paper, the authors substituted the binder; and (ii) the obtained values in the presented papers [
13,
15] are comparable to the values obtained in this current study.
A buildability test was performed to assess the printing potential for real-scale verification. It should be noted that the results from the printing test show a linear correlation with the green strength results.
Figure 15 illustrates a comparison between the height of the printed structure and the green strength results (measured after 30 min of water contact). These results align with those presented in
Figure 7, which show a decrease in static yield stress by adding the fine recycled aggregate (fRA). The samples with an increasing recycled aggregate content and decreasing cement content exhibit a noticeable decrease in the static yield stress growth. However, due to noticeable alterations in the rheological properties of mixes containing fRA, the quality of the material strongly tends to decrease when the fRA content exceeds 20 vol%. Therefore, certain modifications of mix designs and printing process (i.e., slower printing speed) might be required for mixes R30–R50 to ensure the proper quality of printed structures.
The setting time of the mix was evaluated based on the dynamic elastic modulus. The results showed a rapid increase in mechanical properties (initial build-up of E
dyn) starting after about 5 h and 30 min for mixes R0 and R10, which could be assumed as the final setting time. This time aligns with the time presented in [
52] (5.33 h) and is slightly lower than the time presented in this study [
53] (7 h and 10 min). For mixes R20–R50, the rapid increase in mechanical properties is delayed (up to 13 h and 30 min for the R50 mix). This phenomenon is related to the increase in the amount of recycled aggregate in the mix, consistent with studies [
54,
55].
The open porosity analysis revealed a substantial increase in open porosity, due to the reduction in cement content, rising from 2.84% (R0) to 11.36% (R50). This trend of increased porosity due to the mentioned substitution aligns with findings presented in the literature [
56,
57,
58]. However, it is essential to note that different papers have reported varying changes in the porosity for similar substitutions. For example, Guo et al. in 2013 [
56] demonstrated that the porosity increased from 12% to 14% for mixes with a 50% substitution of recycled aggregate (only aggregate substitution, the mix with a cement content of 426 kg/m
3). Muda et al. [
58] showed an increase in the porosity from 37% to 43% with a 50% substitution of aggregate (only aggregate substitution, the mix with a cement content equal to 350 kg/m
3). Anastasiou et al., in 2013 [
57] substituted the cement content with recycled aggregate up to 50% and observed an increase in the porosity from 13% to 21% (the cement content in the reference mix was equal to 350 kg/m
3). It is worth noting that Guo et al. [
56] and Muda et al. [
58] only substituted the aggregate with recycled material, while Anastasiou et al. [
57] replaced the cement (up to 50%) with recycled aggregate. Nevertheless, both sets of studies [
56,
57,
58] demonstrate a significant increase in porosity.
The correlation between oven-dry density and open porosity was established (
Figure 16), confirming an approximately linear relationship. Similar observations were made for compressive strength and open porosity, affirming the state-of-the-art understanding that porosity has a linear relationship with the compressive strength of composites. From this perspective, replacing cement with fine recycled aggregates (fRA) up to 20% by volume seems to be the most reasonable, as the mechanical strength loss was found to be marginal for mixes R10 and R20. In contrast, the higher replacement rates resulted in noticeable strength deterioration. However, considering that 3D printed concrete mixes are generally regarded as high-performance materials, the R50 specimen exhibited a compressive strength of over 40 MPa, indicating a satisfactory mechanical performance to be considered as a structural material [
30,
53,
59].
5. Conclusions
This paper concerned the development of sustainable mortars for 3D printing, aiming at maximum environmental efficiency. In order to achieve this, partial replacements of cement with fine high-quality recycled aggregates produced from 3D printed concrete rejects were attempted. This paper concerns an analysis of the raw materials; mortar development, including fresh and hardened state testing; life cycle assessment to determine the life cycle costs and environmental impacts; and printing runs to evaluate the suitability of the mortars for 3D printing. The following was found:
It is possible to successfully print mixes with up to 50% cement replacement using fine recycled aggregates (fRA) obtained from waste 3D printed concrete elements. However, specimens with 50% cement replacement have some technical drawbacks (see points below).
Adding fRA instead of cement increased the aggregate-to-binder ratio (a/b) from a/b = 1.58 to a/b = 2.86. This phenomenon resulted in the deterioration of the fresh properties of the mix. As the a/b ratio increased, the green strength, static yield stress, and buildability decreased.
This research demonstrates a correlation between the green strength determined by the UUCT test, the buildability during printing, and the static yield stress in the mixes containing fRA. As the static UUCT increased, it became possible to print taller structures, indicating a linear relationship between these properties. The green strength results from the UUCT testing, which are directly linked to buildability during printing, aligned with these findings. The tests indicated that incorporating fRA reduced the green strength by up to 71.9% (for the R50 mix). This correlation is also supported by the static yield stress measured in rheometric research.
The dynamic elastic modulus test indicated that the hardening process was delayed in the mixes with a high fRA content. This phenomenon was also confirmed by a significant reduction in the mechanical properties observed after two days of water contact (up to a 67.62% reduction compared to the reference mix).
Increasing the addition of fRA content led to a decrease in the quality of the mix, resulting in visible defects in the samples.
The open porosity of the mix increased with the addition of fRA, from 2.84% (R0) to 11.36% (R50). This research shows a linear relationship between open porosity and mechanical properties.
Incorporating fRA significantly reduced the hardened mechanical properties, particularly during the initial curing stages. However, by the 28th day, the R50 mix showed a compressive and flexural strength reduction of up to 49.3% and 41%, respectively. Nevertheless, the R50 mix still demonstrated relatively high mechanical properties ( = 41.61 MPa after 28 days and = 5.11 MPa after 28 days), which are sufficient for the structural application of the designed materials.
The LCA analysis showed that reducing the cement content and increasing fRA addition resulted in a significant reduction in mix cost (up to 24%) and a substantial decrease in CO2 emissions (up to 48%). It is worth noting that even in mixes with low fRA content, where there was a limited reduction in green strength (replacement ratios of cement with fRA of up to 30%), the environmental impact of the mix was very promising. For instance, in the R30 mix, the CO2 emissions were reduced by 29% and the cost decreased by 14%.
The research presented in the paper demonstrates that replacing cement with fRA is a promising idea. Although incorporating fRA reduces the green properties of the 3DPC, this approach aligns with sustainable development goals such as reducing CO2 emissions and preserving natural aggregates. Moreover, using recycled aggregates reduces the overall material costs. However, further efforts are required to optimize or introduce chemical additives for improving buildability, green strength, and hardened properties.