‘Advanced Testing and Characterization of Bituminous Materials ~ Loizos, Partl, Scarpas & Al-adi (eds) © 2009 Taylor & Francis Group, London, ISBN 978-0-415-55854-9. Developing a test method for the accelerated ageing of bituminous mixtures in the laboratory N. Piérard & A. Vanelstraete Belgian Road Research Centre, Brussels, Belgium ABSTRACT: Various standardized test methods for binders are available to simulate in the laboratory both the ageing of bituminous binders during mix manufacture and laying and their ageing on site in a bituminous mixture in service. However, there is currently no stand- ardized test method for the laboratory ageing of an entire bituminous mixture. Research was, therefore, undertaken to develop a test method for the reproducible laboratory ageing of bituminous mixtures in a relatively short time, Materials (mixture, binder, aggregate) were sampled on site during the laying of new surface courses, and ageing tests were performed at 60°C on mixtures in bulk. This contribution will describe the development of the new method and its potentialities. The new method is also compared with the RCAT (Rotating Cylinder Ageing Test, EN 15323) ageing method for binders. 1 INTRODUCTION To simulate the ageing of bituminous mixtures, many tests have been developed on their binders. Some of them make it possible to simulate the ageing process of the binder during mix manufacture and laying (RTFOT, TFOT, ...), while others rather simulate binder ageing ‘once the mixture has been laid on site (RCAT, PAV). Alll these tests have been standardized. However, they have the disadvantage of not investigating the ageing of the entire mixture There is currently no common test method standardized at the European level to simulate mix ageing. Nevertheless, the working groups of CEN TC 227 and 336 have pointed out the need for conditioning methods in assessing the durability of asphalt mixtures. Several labo- ratories are engaged in developing an adequate test, such as the Porot & Bobrisow protocol for recycled asphalt pavement production in the laboratory [Porot et al. 2008} In this context, BRRC has been interested in one particular aspect of the ageing of a bituminous mixture, viz. the effect of oxidation. This phenomenon makes the binder harder and more brittle, and modifies the interface between binder and aggregate. This contribu- tion invites you to discover the method which was developed to simulate in the laboratory the ageing process of a mixture in a road pavement in service. The method is based on the accelerated ageing of bulk mixtures in an oven at 60°C while monitoring the development of binder characteristics in this process. In a second part, the new method is compared with the RCAT (Rotating Cylinder Ageing Test) ageing method for binders 2. EXPERIMENTAL SETUP 2.1 Development of the ageing method on bulk material To develop this new method, we looked for a test meeting the following criteria: * casy to perform (no exacting equipment required); * not too time-consuming; + no binder flow during testing, ic., the test temperature had to be lower than the softening temperature of the mastic. 1631, Flowmeter 2. Line of oxygen entering the oven 3, Closed metal eylinder 4, Loose asphalt mixture 5. Line of oxygen leaving Figure I. Device used for ageing bulk mixtures at 60°C under a flow of oxygen, ‘Table 1, Compositions of the mixtures laid on the sites at Ohain and in Ghent AC14 (Qype 1)—Ohain ACI0 (type 4)—Ghent Aggregate ‘Type Content Aggregate ‘Type Content ama Sandstone from Lustin 35.07% 6/10 Porphyry 10.0% 27 Porphyry from Bierges 19.76% © 4/6 Porphyry 48.0% 072 Sand from Chaumont 18.76% 0/2 Porphyry 21.8% 072 Sand from Beez 18.76% ofl Fine sand 13.0% Filler Ta 7.65% Filler Ta 1% Binder Bitumen 50/70 5.9% Binder Bitumen 50/70 6.0% ‘To avoid binder flow, the test temperature was set at 60°C. ‘To shorten the duration of the test, oxygen was used at first. In view of the reasonable duration of the test under oxygen—as we shall see in Section 3.1.1—and of the markedly easier and safer performance of the test, we then investigated the possibility to conduct mix ageing tests under open air conditions. Ageing tests under oxygen require the use of hermetically sealed cylinders (Fig. 1) through which a flow of oxygen is passed (from bottom to top; flow rate = 15 ml/min). In practice, four cylinders (H = 23 cm and @ = 1] cm) are filled with approximately 1.6 kg of bulk mix- ture and placed in an oven at 60°C. The cylinders are grouped into two separate circuits (irenit 1: Cyll and Cy12; circuit 2: Cyl3 and Cyl4) connected to a feed of oxygen. ‘Ageing tests in open air are performed with the mixture under test spread in cake pans. About 1.2 kg of bulk mixture is spread in each pan (0 = 25 em), to a thickness of 2 to 3 cm, Each pan is then placed in an open ait-ventilated oven maintaining a temperature of 60°C throughout the test. 2.2. Bituminous mixtures and binders The samples tested came from two work sites in Belgium: one at Ohain, the other (a private site) in Ghent. The mixtures sampled were of types AC]4 (type 1) and ACIO (type 4). They were used in surface courses. Their compositions are given in the table below. ‘After compaction on site, the voids contents of these mixtures were 3.8 + 1.3% for the ACI4 (type 1) and 3.5 + 0.9% for the AC10 (type 4). They were close-graded mixtures ‘The binders used were pure bitumens, not polymer-modified bitumens. 164Various samples (bulk material, binders, aggregates) were taken during laying: * loose asphalt mixture: to develop the test method for ageing; + aggregates and binder: to be able to prepare a bulk mixture equivalent to that laid on site, if necessary; + binder: to compare the ageing of binders recovered from the laboratory-aged mixture to that of the same binder aged by the RCAT method. In addition, core samples were taken at regular intervals on both sites with a view to the later validation of the ageing method developed on the bulk mixture, 2.3. Ageing methods for binders To allow comparison of the binders extracted from the aged mixtures with the binder aged in the RCAT, the binders were aged by the RCAT procedure described in standard EN 15323. Each binder (500 g) was first aged at 163°C (RCAT163, 4.0 Vimin air, 235 min, 5 revs/min) to simulate the ageing that occurs during the production and laying of an asphalt mixture (also called short-term ageing, STA). After that, it was aged for 140 h at 90°C (RCAT9O, 1 rev/min) under a flow of oxygen (4.5 Vh O.), to simulate ageing in a pavement in service (also called Jong-term ageing, LTA). 24 Methods of analysis ‘The binders extracted from the laboratory-aged mixtures and the binders aged in the RCAT were characterized. Their technological and rheological properties were evaluated from meas- urements of: needle penetration at 25°C (Pen) according to NBN EN 1426; ring-and-ball softening temperature (TR&B) according to NBN viscosity at 60°C, using the plane-plane method; the complex modulus and the phase angle at 52°C and at the frequencies of 1.6 and 10 Hz, according to EN 14770. The measurements were made during a frequency sweep. BN 1427; The rheological measurements were carried out on a Bohling CVO 120 DSR device. The chemical characteristics (extent of oxidation) were determined with an IR spectrom- eter (Perkin Elmer Spectrum One). The binders were dissolved to a concentration of 75 g of binder/l of CCI,. Each spectrum was normalized (correction of the base line between 1,885 and 459 cm"! and absorbance coefficient of a standard bitumen peak situated between 1,400 and 1,500 cm brought to 1.2). The peak surface areas investigated were * A170 (area comprised between 1,530 and 1,770 cm) indicating the presence of carbonyl functions (ketones, esters, carboxylic acids); + A1030 (area comprised between 1,000 and 1,105.3 cm”) indicating the presence of sulfoxides + Atot summing all modifications recorded between 946 and 1,885 cm? For the bulk mixtures, the binder characteristics were determined on the binder extracted and recovered by the procedures described in NBN EN standards 12697-1 (part B2, continu- ous flow centrifuge) and 12697-3. Only the dissolution method differed from that specified in the standard: the loose mixture was dissolved in toluene for one night, under light stirring. 3 RESULTS AND DISCUSSION 3.1 Ageing tests on bulk mixtures 3.1.1 Tests under oxygen ‘An ageing test on the ACI4 (type 1) mixture in bulk was performed at 60°C under oxygen flow, by the procedure described in Section 2.1. The test lasted 78 days. Coarse aggregate was 165‘Table 2. Technological and rheological characteristics of the binder extracted from the ACI4 (type 1) mixture in bulk aged at 60°C under oxygen for 36 and 78 days, 36d 78d Circuit! Circuit? Circuit | Cirenit 2 og Cy) (B) cy) «yay Pen Gi0mm) 4718 20 18 18 TR&B co S164 66.4 658 Viscosity 60 (Pas) 532 2,683 4,253 3,808 GF, 64, 52°C (kPa) 157 624 96.3 833 GA 52°C (kPa) 70.6 362.0 352.1 326.2 By 22 ©) 797 708 68.7 69.1 Boy 52°C © 760 611 630 636 (a) (b) 2 185 a 8 180 rth 3 core 8 pees 7 SY as ze sian game | § m 1 OEE Atot Be TSAI ESAtICo | & tes 5 oye atot 3c QAO EEA |B 1 Gy Alot & ce ee et ee & 180 SG} Att < 155 ° 150 0 10 2 9 40 50 60 7 1 80 90 Duration (days) Figure 2. Ageing of the ACI4 (type 1) mixture in bulk at 60°C under oxygen: development (a) of the carbonyl functions (A170) and the sulfoxide functions (A1030) and (b) of the total area (Atot) meas- ured in infrared spectrometry on coarse aggregate samples from the various cylinders, sampled very regularly to monitor ageing by infrared analysis. The binder was extracted from the loose mixture and characterized at the beginning of the test and after 36 (Cyl2 and Cyl3) and 78 days (Cyll and Cyl4). The values measured are presented in Table 2. The development of the infrared results is shown in Figures 2a and 2b, From Table 2 and Figures 2a and 2b it appears that * the binder extracted from the mixture aged severely during the test. It became harder, as shown by the decrease in penetration and the phase angle of the rigidity modulus and by the increase in ring-and-ball softening temperature, viscosity, rigidity modulus and oxida- tion peaks (A1700, A1030 and Atot); * The characteristics of the binder extracted after 36 days of ageing already indicate an advanced stage of binder ageing, but the binder has not yet reached its final state: its char- acteristics are still evolving. However, for what concerns the simulation of field ageing, the duration of the test can be shortened. Indeed, Choquet F.C. characterized the binders extracted from the top half centimetre slice of asphalt surface courses' after 6 to 19 years of service [Choquet 1991]. Their needle penetration averaged 23 dmm (with individual values ranging between 14 and 37 dmm). This value is of the same order of magnitude as the 18-20 dmm measured in our test after 36 days of ageing. Futhermore, the chemi- cal characteristics of the binder provide information on the test duration to be specified. ‘The oxidation of the binder (carbonyl functions: A1700 and Atot) progresses very rapidly in the first 15 days and then tends to stabilize at a certain level. For the sulfoxide fune- tions the development is faster (5-10 days), but smaller in amplitude. Since the chemical ‘Voids content lower than 5%, road bitumen of penetration grade 50/70. 166characteristics are correlated to the technological characteristics, the duration of the test can be shortened and reduced to about two weeks, for practical reasons; * the ageing can be considered as reproducible. The IR characteristics are very similar, whichever the cylinder from which samples were taken after a given time (Figs 22—2b) In view of the reasonable duration of the test (about two weeks), we tried to develop it for open-air conditions rather than under oxygen. This would simplify the test procedure (no more need to work with hermetically sealed cylinders) and benefit safety. 3.1.2 Tests under air Further ageing tests at 60°C on the mixtures in bulk were undertaken, this time in ambi- ent air. A first test was performed on a bulk mixture prepared in the laboratory with the composition of the ACI4 (type 1), using the mixing procedure described in standard NBN EN12697-35. The same materials were used in the same mix proportions, except for the filler which was slightly different. A second test was carried out on the AC1O (type 4) mixture sampled on the site in Ghent In both cases’, the bulk mixture spread in several pans was aged in an open air-ventilated ‘oven set at 60°C, by the procedure described in Section 2.1. During the test, the pans were removed one after the other from the oven. The binder contained in the aged bulk mixture was then extracted and recovered for a full determination of its technological, (rheological) and chemical (IR) characteristics. The results are presented in Tables 3 and 4. In both cases, the binder contained in the mixtures aged at 60°C in open air aged rapidly: within 5 days, the penetration of the binder from the ACI4 (type 1) mixture decreased by 20. dmm, while that of the binder from the AC10 (type 4) decreased by 16 and 20 dmm after Table 3. Development of the technological and IR (oxidation peak) characteristics of the binder extracted from the ACI4 (type 1) mixture in bulk aged at 60°C in open air Duration (.) Pen (1/10mm) — TR&B(*C)—A1700(em*)—A1030(em") tot Gem) 0 a 53.0 123 40 155.2 10 36 35.7 147 44 162.9 42 29 58.6 165 47 170.0 5.0 20 58.7 169 47 ma Table 4, Development of the technological, chemical, and rheological characteristics of the binders extracted from the ACIO (type 4) mixture in bulk aged at 60°C in open air. sxc Duration Pen TR&B A1700 A1030 Alot Visco 60°C Gg, Goan Seu Som @) 0mm) CQ Com) Com) Com) Pas) (kPa) Pa)" 0 40 54.5 12.6 39 187.7) 711 18.4 85.3 78 78 cor 34 565 134421608968 m5 Ol 77 74 31 0 592 154456781412 3471469757 81 4 614 167 48 ©1722-2066 «= 48220357369 16120 642 187 54 18033159 69.2DISA 7166 Prior to the test on the loose mixture prepared in the laboratory a treatment was necessary, as the freshly manufactured mixture did not exhibit a sufficient extent of ageing comparable to that of the ‘bulk mixture sampled on site, The procedure used for this treatment was based on AASIITO procedure 30-1, It consisted in placing several pans containing the bulk mixture spread to a thickness of 2 to 3.em in an oven at 135°C, to simulate short-term ageing, The duration of this treatment was limited to 75 minutes (instead of the planned 4 hours), since by that time the binder had reached the IR charac- teristics of the bulk mixture sampled on site. After this prior ageing, the various pans were aged in open air in an oven at 60°C, 1678 and 16 days, respectively. This decrease was invariably attended by an increase in ring- and-ball softening temperature and in the intensity of the oxidation peaks (A1700, A1030 and Atot). The developments of the rigidity modulus and the phase angle corroborated this ageing, ‘When comparing the technological and chemical characteristics of the two mixtures aged at 60°C in open air, it can be seen that: * five days of testing are not enough to reach the stage where the ageing kinetics slows down considerably. It is more advisable to extend the duration of the test to 10 days or even two weeks to have an overall idea of the ageing process of the mixture; # ageing seems to be slower for the AC10 (type 4) mixture in bulk than for the AC14 (type 1) mixture. This suggests that the method is capable of revealing composition and materials- related differences in ageing behaviour between mixtures The results of these two open-air ageing tests show that it is possible to age a bulk bitumi- nous mixture in the laboratory so as to simulate the ageing of this mixture in a road pavement in service. The test developed is not too time-consuming, does not require a costly investment and produces considerable quantities of aged mixture. Compared to the method discussed in 3.1.1, it can be shown that this method in air leads to a faster ageing of the bituminous mixture. However, it is premature to draw conclusions about this. The fillers used in AC14 mixture (that was studied according the both methods) were slightly different. This could have influenced the results. 3.2. Comparison of the open-air ageing test at 60°C ‘for mixtures with the RCAT for binders Itis interesting to compare this ageing test for mixtures in bulk with a standardized ageing test for binders, such as the RCAT (EN 15323). The binders of the two mixtures investigated above were, therefore, aged by the RCAT procedure—first at 163°C and then at 90°C, to simulate short-term and long-term ageing, Samples of the binder taken during the test made it possible to monitor the progress of binder ageing for the technological, (rheological) and IR characteristics. Figure 4 shows comparative plots of the characteristics of the binders extracted and recovered from the loose mixture aged at 60°C in open ait and those of the corresponding binders aged at 90°C in the RCAT (LTA), Tt can be seen that + during the first days of testing (3 to 5 days, depending on the mixture) the tech- nological characteristics and the sulfoxide functions of the binders extracted from the mixtures in bulk (AC14 and AC10) developed in a similar way as for the same binders aged at 90°C in the RCAT. Note that for the AC10 (type 4) mixture a shift is (b) 38 So B8 ao Epi § 15 =-ActoPen a gle) we Actavtt —-Acto-Atot 20 |cacteran xo & & — Saran fg otnader aed Figure 3, ‘Comparison of the development of the (a) technological and (b) IR characteristics of the ACI4 (type 1) and AC10 (type 4) mixtures in bulk aged in open air in an oven at 60°C. 1682 50 nm 45 6s E16 ar co Sag Ess sg 8 es SS Be = ATTO0-Bindor_RCATBO 22 Se zt S-A1T00-Bulk- 60°C E20 be 28 “A A1030-Binder_RCATBO = —ePonsinserecatso 4 Bg Noss care gis = Pen-Bulk. 60°C sr OS B10 “#-TREB-Binder RCATIO 30 34 5 TR8B-Bulk 60°C. 28 2? ° a fo 0 42 3 4 5 6 7 o 4 23 4 5 6 7 Duration (days) Duration (days) 225 200 - {6-Bindor_ RCATBO 2-G16-Buk 60°C “t-G0-Binder RCATOO S20 a” — crogule soe 518 ctemsinecpcareo || SpE 8 7s uk Pen Bul #10 SE TRIE Sher ReaTeo | 3° 50 5 SREB Buk GO| 25 25 ° 2 ° o123a45 6788 o 123 45 6 7 8 8 Duration (days) Duration (days) ce ig 16 - == Pe (+ 1700-Binder_ RCATBO gv S-aiToo gui oe 2% = At030.8inder_RCATSO Be == R1030.8uk_60°C so E> Zo 0 123 4 5 6 7 8 8 Duration (days) Figure 4. Development of the technologica, (rheological)! and IR (oxidation peak) characteristics of the binder aged at 90°C in the RCAT and of the binder extracted from the loose mixture aged at 60°C in open air: a) ACI4 (type 1), b) ACIO (type 4) observed (on the y axis) between the initial characteristics of the extracted binder and the binder aged at 163°C in the RCAT. This is due to the ageing of the bulk material sampled on site being less advanced than that obtained by RCAT163 (STA) on the corresponding binder. However, when looking at the shapes of the curves it remains possible to compare the ageing tests on the mixture and the binder, like in the case of the ACI4 (type 1) mixture; + in the longer run, the technological and rheological characteristics of the binders extracted from the aged AC10 mixtures in bulk developed slower than those of the same binder aged at 90°C in the RCAT; ‘* the carbonyl functions (A1700) of the binders extracted from the aged mixtures (ACLO and ACI4) increased faster than those of the binder aged at 90°C in the RCAT. This different behaviour may be explained by the role of the filler in the ageing of a bituminous mixture. There is, indeed, a similarity between the development of the carbonyl functions of the mastic and those of the bulk material aged under the same conditions, while no major change is observed in the sulfoxide functions (Fig. 5). This means that the filler plays a predominant part in the development of the carbonyl functions during the ageing of a bituminous mixture; 16920 18 16 14 & == A1700-Binder_RCATSO + -A1700-Bulk_60°C - E-A1700-Mastic_ 60°C 4 A1030-Binder_RCAT9O ‘A170 and A1030 (-.crm"') e te -\1030-Bulk_60°C 6 = © A1030-Mastic_ 60°C 4 SerrarrTtO 2 0 ° 1 2 8 6 7 Figure 5. Development of the carbonyl (A1700) and sulfoxide (A1030) functions during RCAT90 ageing of the binder and during the ageing of the mastic’ in cupels' and of the mixture (ACI4 (type 1)) in bulk, both at 60°C in open air for several days # the ageing tests on the loose mixture in a ventilated oven at 60°C and on the binder in the RCAT at 90°C were relatively similar in duration. However, some “exhaustion” is observed for the ageing process of the binder contained in the mixture when comparing with the binder aged by the RCAT method. The ageing of the mixture is also less advanced than that of the binder in the RCAT. This seems logical: on the one hand, the ageing tempera- ture of the mixture is lower and, on the other, mix ageing at 60°C in open air is a static test—as opposed to the RCAT, which is dynamic. As a result, the film of binder is not constantly renewed and the ageing process is saturated sooner. 4 CONCLUSION This research project has shown that itis possible to age a bulk bituminous mixture in a labo- ratory test which is easy to perform and is not too time-consuming. The method developed consists in spreading the mixture in bulk to a thickness of 2 tot 3 cm in a cake pan and plac- ing it in an open-air ventilated oven at 60°C for about two weeks ‘A method to age bulk asphalt under oxygen flow was also investigated, but is not to be recommended as it is more difficult to implement (because of the need to have hermetically sealed cylinders) and less safe (owing to the use of oxygen). After two weeks of testing, it produces ageing comparable to that observed in surface courses after 8 to 22 years of service. Comparison of the characteristics of the binders extracted from the mixtures aged at 60°C in open air with those of the corresponding binder aged at 90°C in the RCAT has shown that the ageing of the binder in the mixture is very similar to that of the binder in the RCAT dur- ing the first days of testing, but that the ageing process of the binder in the RCAT is faster in the long run. For the future, BRRC is monitoring the ageing on site of the two mixtures on which the ageing test for mixtures was developed. This will permit more accurate comparison of the Prepared with the filler and binder used for this mixture. *3 grammes of mastic (aged at 163°C in the RCAT to simulate short-term ageing) were poured in each of a number of metal cupels to form a film a few millimetres thick. The cupels were placed in a ventilated oven at 60°C. After 1, 2, 3 and 6 jours, one cupel was removed from the oven and the mastic was dissolved in CCI, for an IR analysis of the binder (before the spectrum was taken, the solution was filtered to remove the filler), 170characteristics determined on the laboratory-aged mixtures in bulk with those of the binders extracted from these mixtures in service, and allow further validation of this new test. ACKNOWLEDGEMENTS The authors gratefully acknowledge the federal government for the financial support of this project under contract number CC-CCN 357. In addition the authors wish to thank P. Crabbé and C, Motte for their technical support. REFERENCES AASHTO R30-1:2006, Standard method of test for Mixture Conditioning of Hot-Mix Asphalt. ‘Choquet FC. 1991, The search for an ageing test based on changes in the generic composition of bitumens, Proc. Inter. Symp. Chemistry of Bitumens, $-8 June 1991, Rome, Italy: 788-812. EN 14770:2005, Bitumen and bituminous binders: determination of complex shear modulus and phase angle: dynamic shear rheometer (DSR). EN 15323-2007, Bitumen and bituminous binders Accelerated long-term ageing/conditioning by the rotating cylinder method (RCAT). NBN EN 1426:2007, Bitumen and bituminous binders: determination of needle penetration. NBN EN 1427:2007, Bitumen and bituminous binders: determination of softening point: ring and Ball method. NBN EN 12697-1:2006, Bituminous mixtures—Test methods for hot mix asphalt—Part 1: soluble binder content. NBN EN 12697-3:2005, Bituminous mixtures—Test methods for hot mix asphalt~Part 3: Bitumen recovery: Rotary evaporator. NBN EN12697-35:2004/A1:2007, Bituminous mixtures—Test methods for hot mix asphalt—Part 35: Laboratory mixing. Porat, L. & Bobrisow, L. 2008, Laboratory mixture ageing protocol for RAP production, Proc. Eurobi- twme & Ewrasphalt congress, Copenhaguen, paper 403-006. im