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Construction and Building Materials 237 (2020) 117415

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Construction and Building Materials


journal homepage: www.elsevier.com/locate/conbuildmat

Acrylic surface treatment applied to architectural High-Performance


Concrete (HPC): Identification of potential pitfalls on the way to
long-lasting protection
Tobias Bader a,b,⇑, Roman Lackner a,b
a
Unit of Material Technology, University of Innsbruck, Technikerstraße 13, A-6020 Innsbruck, Austria
b
Christian Doppler Laboratory for Performance-Based Optimization of Binder Composition and Concrete Manufacturing, Technikerstraße 13, A-6020 Innsbruck, Austria

h i g h l i g h t s

 Seven application amounts were investigated by direct & indirect methods.


 Application process can affect colour change resulting from surface treatment.
 Application process can affect its resistance against weathering.
 Weatherability is characterised by discolouration and delamination.
 Colour differences described by DIN99 and CIELAB colour space are similar.

a r t i c l e i n f o a b s t r a c t

Article history: Surface treatment is recommended for the protection of High-Performance Concrete (HPC) against weath-
Received 27 May 2019 ering. This laboratory study highlighted the underlying weathering mechanisms of treated HPC surfaces
Received in revised form 4 October 2019 when cyclically exposed to UV irradiation and condensation. The extent of the weathering-induced
Accepted 27 October 2019
changes in colour of the acrylic films (perceived as opacity of former transparent films) were revealed
to depend on the application amount (associated with film toughness) and the application method (asso-
ciated with film quality). To ensure long-lasting protection through surface treatment, the films have to
Keywords:
be free of pinholes and sufficiently thick in order to withstand stresses resulting from weathering.
Architectural concrete
High-Performance Concrete (HPC)
Ó 2019 Elsevier Ltd. All rights reserved.
Surface treatment
Coating
Application
Weathering
Colour change

1. Introduction growing interest in the use of HPC for architectural purposes


demands among others the preservation of the original appear-
The term High-Performance Concrete (HPC) describes a type of ance. However, the long-term stability of the aesthetic appearance
concrete that is usually more durable than ordinary concrete of architectural concrete surfaces can be diminished by the envi-
(OC) due to its dense microstructure and very low permeability ronmental conditions they are exposed to (e.g. rain, fog, dew, and
[1]. This circumstance makes HPC from a structural point of view solar radiation). Common types of degradation phenomena, which
interesting for the use in harsh service environments. From an aes- negatively affect the visual perception (e.g. efflorescence, staining)
thetic point of view, the HPC mix design (low water/binder ratio, are triggered by water penetrating HPC superficially [5–8]
fillers and addition of superplasticizers) allows to produce surfaces (see Fig. 1).
that cannot be achieved by conventional mix designs varying from In practice, a common way to prevent effectively the penetra-
smooth (roughness < 1 mm) up to microtextured [2–4]. The tion of water is by applying surface treatment that can prolong
the service life of structural and architectural concrete (e.g. [9–
13]). Although the water absorption of HPC is low, several studies
⇑ Corresponding author at: Unit of Material Technology, University of Innsbruck, highlighted that surface treatment is recommended for HPC (e.g.
Technikerstraße 13, A-6020 Innsbruck, Austria. [14–17]). The requirements on surface treatment applied to
E-mail address: tobias.bader@uibk.ac.at (T. Bader).

https://doi.org/10.1016/j.conbuildmat.2019.117415
0950-0618/Ó 2019 Elsevier Ltd. All rights reserved.
2 T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415

Fig. 1. Schematic illustration of environmental conditions (rain, fog, solar radiation) affecting architectural concrete surfaces by promoting the formation of efflorescence at
the surface and/or staining within the near-surface pores.

architectural HPC differ from structural HPC since architectural the weathering conditions of real building facades that lead to the
surfaces are permanently exposed to view making colour stability formation of undesirable efflorescence [6]. To assess the influence
an important selection criteria. Acrylic coating formulations of artificial weathering on the performance of different application
exhibiting a matt finish may satisfy this demand by avoiding the amounts, both, direct (scanning electron microscopy (SEM),
loss of the mineral appearance of HPC due to the high gloss finish Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction
of conventional formulations [16,18]. (XRD)) and indirect methods (colourimetry) are employed. Addi-
On the way to long-lasting protection of HPC through surface tionally, the influence of the selected colour space (CIELAB,
treatment, the influence of surface properties (e.g. age [3,14], cur- DIN99) on changes in colour due to application of surface treat-
ing condition [3], moisture content [19], surface free energy ment as well as artificial weathering will be evaluated.
[17,20], type of mould [3,4,21]) and surface preparation (e.g. clean- Based on the provided experimental basis, the weathering-
ing [21], sandblasting [3]) were already discussed in literature. induced degradation mechanisms of acrylic surface treatment as
While studies focusing on the longetivity of acrylic surface treat- well as the influence of the application process on the service life
ment within the service environment of building facades are lim- are outlined and guidelines for the proper application of surface
ited to Kozak [44], with the mechanisms leading to the visual treatment according to the protection desired are given in order
deterioration of acrylic surface treatment being unknown. More- to avoid misapplication requiring expensive and time consuming
over, the influence of the application process on the service life maintenance work.
of acrylic surface treatment under the exposure conditions of
building facades remains unclear. Consequently, the objective of
this study is to assess the underlying weathering mechanisms of 2. Materials and sample preparation
acrylic surface treatment and its effect on the visual degradation
of treated HPC surfaces. The so-obtained insights will be beneficial 2.1. Concrete and coating
to evaluate the influence of the application process on the durabil-
ity of surface treatment in the service environment of building The employed mid-grey-coloured HPC substrate is composed of
facades. This is of great importance because the influence of the Ordinary Portland Cement (OPC) CEM I 42.5 R, silica fume, meta-
application process on weatherability of surface treatment is not kaolin, calcareous crushed sand and admixtures (two superplasti-
immediately obvious. cizers, retarder and air entraining agent), see [19]. The used
For this purpose, an artificial weathering environment is water-binder (w/b) ratio for the mix design is 0.33. The maximum
employed that allows reproducing natural weathering within size of calcareous crushed sand is 0.8 mm. The porosimetric details
shorter time by cyclical exposition to solar radiation in the critical and the mechanical properties are given in [15].
short wavelength UV region and condensation. Moreover, the A supplied water-borne acrylic coating (major components:
inclined specimen position (promoting the simulation of rainwater butyl acrylate and methyl methacrylate) with matt finish was
runoff) and the cyclical exposition to wet and dry periods simulate applied. This coating formulation is approved for the protection
T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415 3

Table 1
Physical and chemical properties of the used acrylic coating [19].

Characteristics Details
volume of non-volatile matter 20.0%
major components butyl acrylate, methyl methacrylate
density at 23 °C and 50% RH 1.02 g/cm3
viscosity at 20 °C 403 ± 7 mPa s
glass-transition-temperature of acrylic dispersion 5.0 °C

of concrete [16]. A summary of physical and chemical properties of Table 2


the used coating is given in Table 1. Applied amount of coating in g/m2 for specimens I to III of each test series.

test series specimen I specimen II specimen III


2.2. Preparation of samples HPC + 10 g/m 2
13 9 11
HPC + 20 g/m2 22 23 27
The HPC specimens were older than 28 days and HPC + 30 g/m2 32 28 34
105 mm  75 mm  13 mm in size. One test series consisted of HPC + 40 g/m2 41 38 44
HPC + 60 g/m2 55 61 55
three specimens (specimens named I to III), which were exposed
HPC + 80 g/m2 70 66 90
to artificial weathering. Prior to application of surface treatment, HPC + 100 g/m2 107 121 97
the near-surface substrate moisture content was adjusted to
4 wt-% (procedure is described in [19]) and verified by the mois-
ture tester Hi-520 (Kett Electric Laboratory, Japan). The experimen- (50 mm diameter), three times each (average value was used for
tal program of this study covers coating amounts between 10 and each specimen configuration).
100 g/m2. Up to 40 g/m2, the application varied in steps of 10 g/m2 To monitor the effect of application amount and artificial
and from 40 to 100 g/m2 in steps of 20 g/m2. weathering on the appearance, the total colour difference DE*
Application of the coating was performed in one-step at ambi- was calculated from the brightness L* (100 = white, 0 = black),
ent temperature using a robotic airless spray painting system of the red-green constituent a* (positive = red, negative = green) and
industrial standards with different hydraulic pressure settings at the yellow-blue constituent b* (positive = yellow, negative = blue)
constant spray distance. The underlying pressure settings were coordinates of the CIE 1976 L*a*b* (CIELAB) colour space [23]. For
adjusted based on a control specimen, which was weighted before the DIN99 colour space, the obtained CIELAB colour coordinates
and after coating application in order to determine the applied were transformed according to the procedure described in [24]
amount of coating (= difference in weight) for the individual pres- with the parametric factor kE being set to 1. The corresponding col-
sure settings. Furthermore, the applied amount was confirmed by our coordinates are named L99*, a99* and b99*. Afterwards, DE* was
weighing each specimen before and after surface treatment. calculated for both colour spaces from the differences of each col-
Directly after application of the coating, the specimens were dried our coordinate before and after application of the treatment as well
at 40 °C for 20 min in order to facilitate film formation. The consid- as before and after each interval of artificial weathering, respec-
ered specimens are listed in Table 2 providing the applied amount tively, according to:
of coating. Additionally, three untreated HPC specimens were used DE* = (DL*2 + Da*2 + Db*2)1/2
as reference.

3.2. Scanning electron microscopy (SEM)


2.3. Artificial weathering
For SEM analysis, the scanning electron microscope Quanta 3D
Artificial weathering was performed with the help of the accel- 200i DualBeam (FEI company, Netherlands) was used. Data acqui-
erated weathering tester QUV spray (Q-Lab Cooperation, USA). sition was performed with the help of the xTm 1.72 software.
Specimens were placed in inclined frames, which allowed weath- Acceleration voltage of 25 kV with a current of 1.2 nA was used
ering of spots with 95  65 mm in size. The weathering procedure in low vacuum mode. Image analysis was performed with ImageJ
was set according to EN 4892-3:2006 [22] by cyclical exposition to 1.49v in order to calculate the percentage of HPC surface covered
UV for 8 h (simulating sunlight in the critical short wavelength UV by surface treatment. For this purpose, five backscattered electron
region between 365 nm and solar cut off of 295 nm) at 60 °C as (BSE) micrographs per specimen were analysed. No specific prepa-
well as condensation of deionized water at 50 °C for 4 h. The dura- ration of the specimens was performed before SEM analysis in low
tion of a testing interval (=data point) was 720 h (30 days). In total, vacuum mode.
three intervals were performed amounting to a total weathering
time of 2160 h (90 days). Specimens were repositioned every
3.3. Fourier-transform infrared (FTIR) spectroscopy
120 h in order to ensure equal irradiation. Before performing ana-
lytical experiments, specimens were dried at 40 °C for 4 h.
FTIR measurements were performed with the Alpha (BRUKER,
USA) spectrometer equipped with a single reflection diamond
3. Methods attenuated total reflection (ATR) module in order to evaluate the
coating degradation in the course of artificial weathering. Data
3.1. Colourimetry acquisition was performed using the OPUS 7.5 software. The back-
ground was collected at ambient atmosphere before each measure-
The measurements were conducted with the Chroma Meter CR- ment. The measurements were performed with 128 scans in ATR
410 (Konica Minolta, Japan) using D65 illuminant condition (med- mode in the range of 4000 – 400 cm 1 (resolution of 4 cm 1).
ium daylight) with an observer angle of 2°. The software used for The ATR mode allows obtaining spectra from the surface of the
data acquisition was SpectraMagic NX – Colour Data Software specimens without specific preparation [25].The obtained spectra
CM-S100W V2.5. Each specimen was measured at two spots were baseline corrected, smoothed and normalised to the absorp-
4 T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415

tion band at 1136 cm 1 that was reported by Allen et al. [26] to transformation, the formula giving the colour difference is similar
show marginal changes during photodegradation. to CIE76. Subsequently, the influence of the selected colour space
on colour change resulting from the application of surface treat-
ment will be compared and discussed.
3.4. X-ray diffraction (XRD)
The colour coordinates for both colour spaces (L76*, a76*, b76*;
L99*, a99*, b99*) assessing the investigated mid-grey-coloured HPC
X-ray diffraction (XRD) analysis of efflorescence was performed
surface as well as colour change (expressed by DE76*, DE99*) due
with Empyrean (Panalytical, Netherlands) working with graphite-
to application of the different coating amounts are listed in Table 3.
crystal-monochromatized Cu-Ka radiation generated at 40 kV
As regards DE* various studies have reported different thresholds
and 40 mA. Spectra were taken from 5 to 70° 2 theta with a step
below which colour change is considered acceptable [30,31]. In
size of 0.013° and a counting time of 40 sec/step. Efflorescence
case minimal changes in aesthetic appearance are desired (e.g.
was carefully removed from the weathered HPC surfaces and mea-
architectural surfaces) the refined criterion given by Barath et al.
sured with Si low background sample holders. The software for
may be applied, describing DE* values > 2.0 as undesirable [32].
data acquisition was HighScore Plus V 3.0.5 using PDF-2 database.
Regardless of the colour space used, the observed changes in
colour are mainly due to an increase in L* with marginal changes
4. Results and discussion for the colour components. The transformation of the CIELAB col-
our coordinates by using the DIN99 formula mainly influenced L*
The aesthetic requirements (e.g. colour) on architectural con- as observed by an increase of L*. As expected for the mid-grey-
crete surfaces are higher compared to structural concrete. As the coloured HPC surface with no apparent hue, the changes of a*
human perception of colour is subjective, instrumental colour and b* due to transformation are negligible. Colour changes
measurement is used to express colour by means of colour coordi- expressed by DE76* and DE99*, respectively, revealed similar ten-
nates within a colour space. Based on the colour coordinates, dencies – an increase in colour change with increasing application
changes in colour are assessed by using a colour-difference for- amount. Hence, the influence of the selected colour space on the
mula. However, perceptual non-uniformities in the commonly assessment of colour changes resulting from acrylic surface treat-
used CIELAB colour space are reported to affect the colour differ- ment are regarded as marginal.
ence (e.g. [27,28]). Today well-known approaches to compensate The observed increase in L* of treated HPC surfaces is attributed
this circumstance are either the modification of the colour differ- to the matt finish of the used formulation since clear solutions of
ence formula (e.g. CIE94 and CIEDE2000 [29]) or the transforma- acrylic surface treatment are reported to cause a decrease in L*
tion of the entire colour space (DIN99 [24]). In case of the DIN99 [33]. As reported in our previous study [16], the changes in colour

Table 3
Colour coordinates (CIE76, DIN99) of untreated and treated mid-grey-coloured HPC surfaces before (interval 0) and after each interval of artificial weathering as well as colour
change (DE*) resulting from application of acrylic coating (HPC + 10 until HPC + 100 g/m2) and artificial weathering. Mean value and standard deviation were obtained from 18
measurements each and colour differences were calculated for the individual intervals with respect to colour coordinates of interval 0. In case of treated HPC surfaces, the colour
coordinates of the untreated specimens is similar to the reference HPC specimen. Optical photos are given as supplementary data.

test series interval L76* [–] L99* [–] a76* [–] a99* [–] b76* [–] b99* [–] DE76* [–] DE99* [–]
HPC (untreated) 0 39.1 ± 0.2 50.8 ± 0.2 0.4 ± 0.0 0.4 ± 0.0 2.8 ± 0.1 1.9 ± 0.1 – –
1 53.0 ± 0.3 64.2 ± 0.3 0.1 ± 0.0 0.5 ± 0.1 2.2 ± 0.1 1.5 ± 0.1 13.9 ± 0.3 13.4 ± 0.3
2 54.3 ± 0.3 65.4 ± 0.3 0.2 ± 0.0 0.4 ± 0.1 2.0 ± 0.1 1.4 ± 0.1 15.2 ± 0.3 14.6 ± 0.3
3 54.9 ± 0.2 65.9 ± 0.2 0.2 ± 0.0 0.3 ± 0.1 1.9 ± 0.1 1.3 ± 0.1 15.8 ± 0.3 15.1 ± 0.3
HPC + 10 g/m2 0 41.9 ± 0.2 53.6 ± 0.2 0.2 ± 0.0 0.6 ± 0.0 2.9 ± 0.0 1.9 ± 0.0 2.6 ± 0.3 2.6 ± 0.3
1 52.3 ± 0.4 63.5 ± 0.4 0.1 ± 0.0 0.6 ± 0.0 2.5 ± 0.0 1.6 ± 0.0 10.4 ± 0.5 9.9 ± 0.4
2 54.8 ± 0.1 65.8 ± 0.1 0.1 ± 0.0 0.4 ± 0.0 2.0 ± 0.1 1.3 ± 0.0 13.0 ± 0.2 12.2 ± 0.2
3 55.2 ± 0.1 66.2 ± 0.1 0.1 ± 0.0 0.3 ± 0.0 1.8 ± 0.1 1.2 ± 0.1 13.4 ± 0.2 12.6 ± 0.2
HPC + 20 g/m2 0 43.2 ± 0.2 54.9 ± 0.2 0.2 ± 0.0 0.6 ± 0.0 2.8 ± 0.1 1.9 ± 0.1 4.1 ± 0.4 4.2 ± 0.4
1 47.6 ± 1.1 59.2 ± 1.1 0.0 ± 0.1 0.9 ± 0.1 3.4 ± 0.3 2.2 ± 0.2 4.5 ± 1.1 4.3 ± 1.0
2 52.9 ± 1.2 64.1 ± 1.1 0.1 ± 0.1 1.0 ± 0.1 3.3 ± 0.2 2.1 ± 0.1 9.7 ± 1.0 9.2 ± 0.9
3 57.9 ± 0.9 68.2 ± 0.8 0.4 ± 0.0 1.2 ± 0.1 3.4 ± 0.1 2.1 ± 0.1 14.8 ± 0.7 13.7 ± 0.6
HPC + 30 g/m2 0 44.1 ± 0.7 55.7 ± 0.7 0.2 ± 0.0 0.6 ± 0.0 2.8 ± 0.1 1.9 ± 0.1 4.9 ± 0.8 4.9 ± 0.7
1 46.9 ± 1.0 58.5 ± 0.9 0.1 ± 0.1 0.8 ± 0.1 3.2 ± 0.2 2.0 ± 0.1 2.9 ± 1.2 2.8 ± 1.1
2 55.2 ± 2.3 66.2 ± 2.0 0.3 ± 0.1 1.1 ± 0.2 3.5 ± 0.3 2.2 ± 0.1 11.2 ± 2.0 10.5 ± 1.7
3 59.6 ± 1.2 70.0 ± 1.0 0.4 ± 0.1 1.2 ± 0.1 3.3 ± 0.2 2.0 ± 0.1 15.6 ± 1.2 14.3 ± 1.0
HPC + 40 g/m2 0 44.4 ± 0.6 56.1 ± 0.5 0.2 ± 0.0 0.5 ± 0.0 2.6 ± 0.0 1.7 ± 0.0 5.7 ± 0.6 5.7 ± 0.5
1 44.9 ± 0.7 56.6 ± 0.6 0.1 ± 0.0 0.7 ± 0.1 3.1 ± 0.2 2.0 ± 0.1 0.7 ± 0.3 0.6 ± 0.3
2 57.5 ± 1.9 68.2 ± 1.7 0.2 ± 0.1 1.0 ± 0.2 3.0 ± 0.3 1.9 ± 0.2 13.1 ± 1.6 12.1 ± 1.3
3 61.8 ± 1.9 71.9 ± 1.6 0.3 ± 0.1 1.0 ± 0.2 2.8 ± 0.4 1.8 ± 0.2 17.4 ± 2.2 15.8 ± 1.9
HPC + 60 g/m2 0 44.7 ± 0.5 56.4 ± 0.4 0.2 ± 0.0 0.5 ± 0.0 2.6 ± 0.1 1.7 ± 0.0 6.2 ± 0.5 6.2 ± 0.5
1 44.2 ± 0.4 55.9 ± 0.4 0.2 ± 0.0 0.4 ± 0.0 2.9 ± 0.2 1.7 ± 0.0 0.6 ± 0.4 0.5 ± 0.4
2 57.5 ± 2.2 68.1 ± 1.9 0.2 ± 0.1 1.0 ± 0.2 3.1 ± 0.4 2.0 ± 0.2 12.7 ± 2.3 11.7 ± 2.0
3 59.3 ± 2.9 69.7 ± 2.5 0.2 ± 0.1 0.9 ± 0.1 2.6 ± 0.2 1.7 ± 0.1 14.6 ± 2.8 13.3 ± 2.4
HPC + 80 g/m2 0 45.4 ± 0.6 57.1 ± 0.5 0.2 ± 0.0 0.5 ± 0.0 2.7 ± 0.1 1.8 ± 0.0 6.6 ± 0.9 6.6 ± 0.9
1 45.1 ± 0.4 56.8 ± 0.4 0.2 ± 0.0 0.5 ± 0.1 2.7 ± 0.1 1.8 ± 0.1 0.3 ± 0.3 0.3 ± 0.3
2 52.1 ± 1.6 63.4 ± 1.5 0.0 ± 0.1 0.7 ± 0.1 2.7 ± 0.2 1.7 ± 0.1 6.7 ± 2.1 6.3 ± 1.9
3 58.9 ± 2.6 69.4 ± 2.2 0.2 ± 0.2 0.8 ± 0.2 2.5 ± 0.4 1.6 ± 0.2 13.4 ± 3.0 12.3 ± 2.7
HPC + 100 g/m2 0 45.4 ± 0.3 57.0 ± 0.3 0.2 ± 0.0 0.5 ± 0.0 2.8 ± 0.1 1.9 ± 0.0 6.7 ± 0.4 6.7 ± 0.4
1 45.4 ± 0.4 57.0 ± 0.4 0.2 ± 0.1 0.6 ± 0.1 2.9 ± 0.3 1.9 ± 0.1 0.1 ± 0.1 0.1 ± 0.1
2 45.5 ± 0.2 57.5 ± 0.2 0.2 ± 0.0 0.5 ± 0.0 2.8 ± 0.1 1.8 ± 0.1 0.1 ± 0.1 0.1 ± 0.1
3 49.1 ± 0.6 60.6 ± 0.6 0.0 ± 0.0 0.8 ± 0.1 3.1 ± 0.2 2.0 ± 0.1 3.7 ± 0.7 3.6 ± 0.7
T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415 5

resulting from application of the matt film became appreciable due


to the low L* of the substrate. Hence, an increasing application
amount comes along with an increasing amount of matting agent,
which seems to cause the perceptible increases in L*. However, the
extent of colour change for 100 g/m2 is greater compared to the
equal amount applied by rollers in our previous study
(DE76* = 2.7 ± 0.2 [16]). Consequently, the application method
seems to additionally affect the colour change of HPC induced by
surface treatment. This may be explained by the surface roughness
of the protective film and its interaction with incident light.
Based on the obtained results, we assume that the application
process (amount and method) influences the colour change result-
ing from surface treatment. Although the extent of colour change
decreases with decreasing application amount, the observed
changes in colour are still undesirable according to the refined cri-
terion given by Barath et al.
Fig. 2. Results of XRD analysis of efflorescence salts formed due to exposition to
Both architectural concrete surfaces and applied surface treat- artificial weathering on (a) untreated HPC, (b) HPC + 10 g/m2, (c) HPC + 20 g/m2 and
ment are permanently exposed to weathering, diminishing the (d) HPC + 30 g/m2. (Abbreviation: Cc, calcite; Vtr, vaterite).
aesthetic appearance of architectural concrete surfaces with ongo-
ing weathering time due to e.g. formation of efflorescence (con-
crete) or discolouration (surface treatment). For coatings applied HPC) and the film forming components (remaining on the surface).
to architectural aluminium panels, the American Architectural The investigated HPC surface is characterised by regularly dis-
Manufacturing Association (AAMA) admits a maximum colour tributed rounded asperities (average diameter: 200 – 300 mm)
change of 5.0 due to exposition to weathering (Florida exposure and rounded pores that had diameters in the range between 50
for five years) [34]. The authors regard the mentioned maximum and 250 mm. The coverage of HPC surfaces before and after each
colour change as an appropriate threshold for the evaluation of interval of artificial weathering are given in Fig. 4. Before artificial
the performed artificial weathering experiment. weathering, coating films with incomplete coverage of HPC sur-
Colour coordinates (L76*, a76*, b76*; L99*, a99*, b99*) of untreated faces were observed for films resulting from 10 (40 ± 5%), 20
and treated HPC surfaces after each interval of artificial weathering (86 ± 5%) and 30 g/m2 (88 ± 6%). While the protective films result-
as well as the respective colour changes (DE76*, DE99*) are listed in ing from application of 40 (98 ± 1%), 60 (98 ± 1%), 80 (99%) and
Table 3. 100 g/m2 (100%) covered the HPC surfaces almost completely.
Again, the transformation of the CIELAB colour coordinates by The observed differences in coverage may be attributed to the sub-
using the DIN99 formula mainly influenced L*, giving increased strate that is rough and contains pores. This seems to complicate
values for L*. As expected for the mid-grey-coloured HPC surface the complete coverage of HPC surfaces with small coating
with no apparent hue, the changes for a* and b* are negligible. Col- amounts. Moreover, all films exhibited circular voids varying in
our changes expressed by DE76* and DE99*, respectively, revealed size between 10 and 60 mm, with some voids going completely
similar tendencies: For untreated and treated HPC surfaces the col- through the coating film exposing the underlying HPC surfaces.
our changes resulting from exposition to artificial weathering are The amount of voids as well as voids going completely through
mostly related to an increase in L* with minor changes for a* and the coating film seems to decrease with increasing application
b*. The untreated reference HPC surface showed after interval 1 amount.
remarkable changes in colour, which increased considerably less After interval 1 of artificial weathering, SEM micrographs
after intervals 2 and 3. For the treated HPC surfaces, the extent revealed randomly distributed granular crystals of a few microns
of colour change varied between the different application amounts. on untreated and surfaces treated with 10, 20 and 30 g/m2 due
For 10 g/m2, already after interval 1 remarkable colour change was to weathering. With the help of XRD analysis, the calcium carbon-
observed. For 20 – 80 g/m2 similar colour changes were measured ate polymorph calcite was detected and in addition to calcite, the
after interval 2. Whereas for 100 g/m2, the changes in colour were polymorph vaterite was detected for surfaces treeated with 20
up to interval 2 not appreciable amounting to a colour change < 5.0 and 30 g/m2 (see Fig. 2a–d).
after interval 3. However, in contrast to the previous section the Thus, water arriving at the surface of the mentioned specimens
colour changes expressed by DE99* and DE76* differed slightly. extracted the soluble calcium-bearing constituents from the hard-
The modification of L* by the transformation of the CIELAB colour ened cement paste, which later reacted with carbonic acid (from
coordinates using DIN99 is suspected to cause the observed devia- atmospheric carbon dioxide) to form insoluble calcium carbonate.
tion between DE99* and DE76*. In case of this study, the focus was In case of the treated HPC surfaces, the coating films resulting from
on a maximum colour change of 5.0, hence, the observed variances 10, 20 and 30 g/m2 were not able to prevent efflorescence forma-
between the two colour spaces are regarded as negligible since the tion. This is attributed to the incomplete coverage of HPC surfaces
deviation is not appreciable by the naked eye. that did not stop water from penetrating. While application
To evaluate the underlying cause for the observed changes in amounts  40 g/m2 prevented efflorescence formation by hinder-
colour, SEM, FTIR spectroscopy and XRD analysis are employed. ing water from extracting the soluble calcium-bearing con-
Representative SEM micrographs showing the surface of treated stituents. With ongoing exposition to artificial weathering, the
HPC substrates before and after artificial weathering are given in coverage of HPC surface decreased with the extent of decrease
Fig. 3a–c. depending on the application amount. In case of coating films
In our previous study, we highlighted that the used acrylic coat- resulting from the application of 10 g/m2, a noticeable decrease
ing is not absorbed into the near-surface area of HPC and, thus, in the coverage was already detected after interval 1 that is attrib-
occurs only superficial [19]. This observation is assigned to the uted to delamination. The coverage of HPC further decreases with
reduced porosity and pore size of the near-surface area of the ongoing exposition to artificial weathering suggesting the proceed-
investigated HPC that seem to act as a filter. Thus, the applied ing delamination of the non-continuous films. For 20 – 80 g/m2, the
aqueous dispersion is separated into water (being absorbed by coverage of HPC surface was almost unchanged up to interval 1
6 T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415

Fig. 3. Representative micrographs of HPC surfaces before and after interval 3 of artificial weathering coated with 10 g/m2 (a), 60 g/m2 (b) and 100 g/m2 (c) of the acrylic
coating (dark area = coating, bright area = concrete).

and decreases progressively after intervals 2 and 3, respectively.  The development of a shoulder peak (1815 – 1752 cm 1) on the
The observed decrease in coverage is attributed to cracking and broadened carbonyl ester peak (1720 cm 1), which may be
local spots of delamination. At the end of the artificial weathering attributed to the formation c-lactone structures being most
experiment, the highest residual coverage of HPC was observed for likely caused by cyclisation reactions [26,35–37].
100 g/m2 (average of 95%).  The progressive increase in absorption in the region 3680 –
Additionally, FTIR spectroscopy was employed to assess the 3050 cm 1 suggests the formation of hydroxyl groups that can
alteration of the acrylic coating due to exposition to artificial be associated with the formation of e.g. carboxylic OH groups
weathering, with the exposition to UV radiation causing the pho- as well as with other OH groups such as alcohols or thermal
todegradation of the organic coating. Representative FTIR spectra instable hydroperoxides [35,36]. If hydroperoxides are formed,
comparing the acrylic coating before and after each interval of arti- they will mostlikely decompose immediately due to the exposi-
ficial weathering are given in Fig. 5, showing: tion to UV radiation and heat [38,39].
T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415 7

Fig. 4. Coverage of HPC surfaces by acrylic coating (a) after application of surface treatment and after (b) interval 1, (c) interval 2 and (d) interval 3 of artificial weathering.

ted to the formation of efflorescence (calcium carbonate)


highlighting the necessity of surface treatment for architectural
HPC. After intervals 2 and 3, the increase in colour change was
comparatively lower suggesting that calcium carbonate deposition
closes the open porosity of the surface, which is in accordance with
the results reported by Horgnies et al. [3]. Hence, the extraction of
additional calcium-bearing constituents from the hardened
cement paste was mostlikely reduced. The investigated amounts
of acrylic surface treatment resulted in either incomplete (10, 20
and 30 g/m2) or complete coverage (40, 60, 80 and 100 g/m2) of
HPC surfaces. After three intervals of artificial weathering, the
selected criterion for a maximum colour change of 5.0 due to expo-
sition to weathering was only met by applying 100 g/m2 of the
investigated acrylic surface treatment.
Fig. 5. Representative FTIR-spectra of the applied acrylic coating (application
amount 100 g/m2) before (solid line) as well as after interval 1 (dashed line), The aforementioned differences in the performance between
interval 2 (dash-dotted line) and interval 3 (dotted line) of artificial weathering. the investigated application amounts of acrylic surface treatment
with regard to the long-term stability are discussed in the
following:
 The progressive decrease in the C–H stretching absorption In general, alteration of acrylic surface treatment is a conse-
(3000 – 2850 cm 1) suggests chain scission involving the for- quence of both, ‘substrate-related’ and ‘environmental-related’ pro-
mation of volatile monomer molecules [35]. cesses. In order to minimise the influence of ‘substrate-related’
 The progressive increase in absorption at 1640 cm 1 may be alteration process, we adjusted the substrate moisture content to
attributed to the formation of unsaturated chain-end bonds 4 wt-% [19]. Thus, artificial weathering-induced degradation
(C = C) that can result from chain scission reactions [26,35,36]. (‘env.-rel.’ processes) is suspected to be the primary cause for the
observed alteration of the acrylic surface treatment and changes
The main results of the performed experimental study can be in colour of treated HPC surfaces.
summarized as follows: After exposition to the artificial weathering environment, the
The untreated HPC surfaces exhibited after interval 1 of artifi- changes in colour of treated HPC surfaces were noticeable by an
cial weathering considerable changes in colour, which are attribu- increase in L*. For 10, 20 and 30 g/m2, these changes in colour
8 T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415

are attributed to both calcium carbonate efflorescence and dis- coating is suspected to induce additional loading, causing cracking
colouration of the coating. In case of HPC treated with application and delamination of the brittle coating films.
amounts 40 g/m2, no efflorescence deposition was observed. This Moreover, it is supposed that the interaction between the inves-
is attributed to complete coverage of HPC surface by the protective tigated coating films and the artificial weathering environment
films hindering water from entering, while carbon dioxide most was additionally influenced by the underlying application method.
likely can pass through the film to form calcium carbonate within In this study, the coating deposition was performed by spraying
the near-surface area of concrete. Consequently, the observed whereas in our previous study [19] the application was performed
changes in colour are attributed to the visual deterioration of the by rolling (considering application amounts of 40 and 60 g/m2). In
coating film in the course of artificial weathering. The mentioned contrast to rolling, the coating deposition by spraying resulted in
increase in L* of treated HPC substrates due to discolouration of pinholes (perceived as circular voids). In case of application
acrylic surface treatment is assumed to be initiated by moisture amounts such as 40 and 60 g/m2, certain pinholes extended to
subsequently accumulating within voids of the coating film due the HPC surface that are suspected to weaken the film toughness.
to interactions with polar substances (e.g. surfactants [19]). These These differences in film toughness seem to influence the alter-
voids within the coating – in size greater than the wavelength of ation behaviour (colour change and delamination), which is of
light – cause the subsequent scattering of incident light, creating minor extent for coatings films applied by rolling compared to
opacity and whiteness of the originally transparent acrylic films their pendants applied by spraying.
[40,41]. The presence of these voids, however, is reported to be Based on these observations, we assume that the presence of
controlled by the rigidity of the polymer film [42], with the latter pinholes makes coatings films with insufficient film thickness
being influenced by the film thickness [38]. In case of the present more susceptible to degradation. In case that acrylic surface treat-
study, the investigated different application amounts result in dif- ment will be applied by spraying, it is recommended to apply at
ferent film thicknesses, explaining the observed differences in the least 100 g/m2 in order to achieve the desired colour stability that
extent of opacity of the former transparent films. is one of the aesthetic parameters affecting the overall quality of
Additionally, photodegradation alters the coating by either buildings. By applying 100 g/m2, the risk of misapplication of sur-
breaking chemical bonds directly or forming free radicals, which face treatment resulting in early failure (discolouration and delam-
subsequently facilitate cyclisation and crosslinking reactions ination) can be minimised because the underlying film thickness
[35,36]. We assume that, the detected structural changes of the seems to be sufficient to compensate the influence of possible pin-
used acrylic coating affect the mechanical properties of the film holes as well as the stresses in consequence of ‘environmental-
by e.g. decreasing its deformability (embrittlement) [43,44]. The related’ processes (see Fig. 6).
cyclical exposition to condensation (associated with a wet environ- In general, the application of surface treatment results in addi-
ment) and UV irradiation (associated with a dry environment) tional material costs and an additional working step (labour costs).
seems to cause the permeation of moisture into and out of the The increased initial costs must be balanced against both, the pro-
coating. The underlying repeated swelling and shrinkage of the longed service life of architectural concrete (colour stability) and

Fig. 6. Schematic illustration of ‘application-related’ (e.g. film thickness, pinholes) and ‘environmental-related’ factors (e.g. moisture accumulating within voids, cyclisation
reactions, crosslinking, chain scission) influencing the long-term stability of acrylic surface treatment applied to HPC surfaces under the exposure conditions of building
facades.
T. Bader, R. Lackner / Construction and Building Materials 237 (2020) 117415 9

the avoided costs for the removal of undesirable efflorescence. Our the subsequent accumulation of moisture within the coating
study showed that the application of surface treatment motivated films. These accumulations seem to cause opacity of the former
by cost or appearance can result in a lack of protection or early fail- transparent films (observed by an increase in brightness). The
ure that makes the inexpensive surface treatment far more expen- cyclical exposition to wet and dry environments seems to cause
sive than the amount that lasts a longer period. the permeation of moisture into and out of the coating. The
The time span over which surface treatment has an acceptable underlying repeated swelling and shrinkage of the coating is
appearance and offers adequate protection in its service environ- suspected to induce additional loading, causing cracking and
ment is described by the term service life. The used artificial flaking of the brittle coating films. Based on these observations,
weathering environment was selected in order to assess the the application process was revealed as an important factor
weathering-induced degradation mechanisms occurring at build- influencing the service life of acrylic surface treatment.
ing facades. A reliable statement on how long the applied surface
treatment will last in real outdoor environment based on these Recommendations to ensure long-lasting protection of HPC in
experiments is difficult because the duration and frequency of nat- the service environment of building facades through acrylic surface
ural water cycles as well as the temperature during UV and mois- treatment comprises, on the one hand, sufficient film thickness
ture stresses are primary variables in natural weathering. In (associated with film toughness) and, on the other hand, absence
literature, the service life expectations for acrylic coatings are esti- of pinholes (associated with film quality). Based on the results of
mated with up to 10 years [45], whereas some case studies this experimental study, 100 g/m2 of the investigated acrylic coat-
reported life times of about 20 years under the exposure conditions ing applied by spraying fulfilled these requirements. However, its
of real building facades [12,46]. application resulted in a preceding change in colour of HPC
In general, the results obtained within this study for architec- (DE* > 2.0) making the coating film appreciable with the naked
tural HPC may be transferred to structural HPC. However, harsh eye. Nevertheless, the film thickness resulting from the application
service environments may require application amounts that are of 100 g/m2 was sufficient to encounter the detected
several times higher than the investigated amounts. Thus, is has ‘environmental-related’ stress factors. Hence, the residual percent-
to be taken into account that thick coating films may influence age of HPC surface covered by 100 g/m2 of the used acrylic coating
the underlying film formation process due to the formation of (average 95%) and the detected colour change (DE* < 5.0) after
so-called skins that are reported to cause vertical inhomogeneities 2160 h of artificial weathering were acceptable – fulfilling e.g.
[40,47]. the requirements of the American Architectural Manufacturing
Association that was introduced for architectural aluminium
5. Conclusion panels.

Within the present study, the weathering mechanisms of acrylic Declaration of Competing Interest
surface treatment were highlighted and their effect on the visual
deterioration of treated HPC surfaces was assessed. Based on the The authors declare that they have no known competing finan-
results obtained, the influence of application process on the dura- cial interests or personal relationships that could have appeared
bility of surface treatment in the service environment of building to influence the work reported in this paper.
facades was evaluated. For this purpose, different coating amounts
(10 – 100 g/m2) applied by spraying were exposed to artificial Acknowledgements
weathering (UV radiation, condensation) and analysed with regard
to colour stability and efflorescence prevention by colourimetry, The research results presented in this study were obtained
SEM and FTIR spectroscopy. within the Christian Doppler Laboratory for Performance-Based
From the obtained results the following conclusions can be Optimization of Binder Composition and Concrete Manufacturing
drawn: (University of Innsbruck, Innsbruck, Austria). The financial support
by the Austrian Federal Ministry of Science, Research and Economy
 The application of the investigated acrylic coating with matt and the National Foundation for Research, Technology and Devel-
finish resulted in colour changes of HPC surfaces that were opment as well as the associated industrial partner is gratefully
mainly related to an increase in brightness with marginal acknowledged. The authors are grateful for the assistance of Martin
changes for the colour coordinates. The extent of colour change Wieser and Paul Jäger in the course of the presented research work.
increased with increasing application amount. These changes
are assumed to be caused by the matting effect and the film sur-
face roughness and became visible due to the low L* of the Appendix A. Supplementary data
investigated substrate. The resulting changes in colour
expressed by DE76* and DE99*, respectively, showed similar ten- Supplementary data to this article can be found online at
dencies (DE* > 2.0). Hence, the influence of the underlying col- https://doi.org/10.1016/j.conbuildmat.2019.117415.
our space on the estimation of the detected colour changes for
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