Tire pyrolysis oil in Brazil: Potential production and quality of fuel

Renewable and Sustainable Energy Reviews xxx (xxxx) xxx

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Tire pyrolysis oil in Brazil: Potential production and quality of fuel ~o A. de Carvalho Jr. a Alexander R. Gamboa a, *, Ana M.A. Rocha b, Leila R. dos Santos c, Joa a

S~ ao Paulo State University, UNESP, Guaratinguet� a Campus, FEG, Av. Ariberto P. Cunha, 333, CEP 12516-410, Guaratinguet� a, SP, Brazil Federal University of Ouro Preto - UFOP, School of Mines, EM, R. Diogo de Vasconcelos, 122, Pilar, Ouro Preto, MG, 35400-000, Brazil c Technological Institute of Aeronautics - ITA, Combustion, Propulsion and Energy Laboratory - LCPE., Rod. Praça Marechal Eduardo Gomes, 50, CEP 12228-900, S~ ao Jos�e dos Campos, SP, Brazil b

A R T I C L E I N F O

A B S T R A C T

Keywords: Waste tires Pyrolysis Potential production Tire pyrolysis oil Brazil

The application of tire pyrolysis technology in a country will be feasible whenever competitive and attractive products are produced. In this work, quantitative and qualitative evaluation of the potential of tire pyrolysis oil (TPO) in Brazil was carried out. The quantitative evaluation consisted of determining the amount of feedstock (waste tires) available and the volume of TPO that can be produced in Brazil per year. The qualitative evaluation was applied to a sample of TPO produced in Brazil, determining its main atomization properties: specific mass, viscosity and surface tension. In addition, a theoretical comparison of the quality of TPO spray was performed, comparing the expected mass median diameter for TPO and diesel oil (DO) spray. The results of the quantitative evaluation showed that it is possible to produce around 230 to 280 thousand m3 per year of TPO, equivalent to about 2% of the onshore petroleum and fuel oil (FO) produced in Brazil for both cases. Meanwhile, the quali­ tative evaluation showed that the TPO produced in Brazil has greater ease of atomization in relation to the FO produced and marketed in the country. However, preserving the quality of TPO requires proper storage, since prolonged exposure to the environment increases its viscosity by up to four times, and can change it from me­ dium oil (22.3oAPI) to heavy oil (14.1oAPI).

1. Introduction

2% a year [4]. The literature contains extensive information on the production of TPO from the traditional pyrolysis process [4–8]. Some researchers [9–13] have reported improvements in the production of TPO and its physicochemical properties with the introduction of cata­ lysts in the traditional pyrolysis process. On the other hand, the co-pyrolysis of tires and materials such as grape seeds [11], oily wastes [14], palm shells [15] and bituminous coal [16] has also been investi­ gated. However, the amount of TPO needs to be quantified, especially in countries whose tire production is relevant, like Brazil, which has 20 tire factories [17]. The energy potential of TPO has motivated some researchers to study its use as alternative fuel in furnaces [18,19], boilers [20] and compression ignition engines [21–23], especially in those latter thermal machines [24]. However, high sulfur content (above 0.6% by mass) restricts its direct use [25], but some researchers have been able to remove up to 87.8% of the original sulfur [26]. Another way to reduce sulfur content in TPO and improve its properties (such as cetane num­ ber) is to blend it with other fuels such as biodiesel [22] or diesel [23]. Another important aspect that must be considered in the production of TPO is its use as a source of feedstock to obtain traditional fuels such

The stability of a society depends on several elements and conditions, such as energy resources and balance between development and envi­ ronmental quality. Currently, fossil fuels are the main non-renewable energy resources of the industrial processes that move the world. On the other hand, products introduced to improve living conditions have caused significant changes in the environment. The impact of these products is often due to their slow degradation, which can take hundreds of years. One way to save fossil fuels and mitigate environmental impact is to produce fuels obtained from waste. Waste tires are an attractive source of raw material for fuel production, since large amounts are generated each year [1]. The reuse of waste tires through pyrolysis recycling technology is a good alternative to eliminate waste from the environment and obtain products with high energy value such as py­ rolysis oil, pyrolysis gas and pyrolysis coal [2,3]. The oil obtained from tire pyrolysis, called tire pyrolysis oil (TPO), is an alternative liquid fuel with similar properties to diesel. Large-scale TPO production can become viable since there is a large amount of feedstock available (waste tires) in the world, which increases by around * Corresponding author. E-mail address: [email protected] (A.R. Gamboa).

https://doi.org/10.1016/j.rser.2019.109614 Received 27 May 2019; Received in revised form 16 November 2019; Accepted 18 November 2019 1364-0321/© 2019 Elsevier Ltd. All rights reserved.

Please cite this article as: Alexander R. Gamboa, Renewable and Sustainable Energy Reviews, https://doi.org/10.1016/j.rser.2019.109614

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~ ng, as gasoline and diesel. Simulated distillation of TPO performed by Du et al. [27] showed that it can be fractionated into gasoline (~12 wt%), kerosene (~33 wt%), gasoil or diesel (~34 wt%), fuel oil (~6 wt%) and heavy vacuum oil (~15 wt%), according to the respective boiling tem­ peratures. In the works of Ayanoglu and Yumrutas [28,29], three liquid products of tire pyrolysis were obtained: wax, heavy oil and light oil. Heavy oil and light oil were obtained from the condensation of pyrolysis vapors by two heat exchangers operating in the temperature range of 100–250 � C and 75–200 � C, respectively. The H and C contents in light and heavy oils were similar to that of standard fuels (gasoline and diesel), while the contents of N and S were higher. On the other hand, physical properties like density and viscosity of heavy and light oil were very close to those of standard petroleum fuel. Research shows the viability of TPO production and the attractive properties that it possesses for direct use in thermal equipment or to obtain alternative fuels similar traditional ones. However, there is no detailed information on the amount of feedstock available (waste tires) and the potential annual production of TPO in countries with large populations such as Brazil1 (over 200 million people). This information was corroborated in the Web of Science platform, which revealed that Brazil until 2018 has produced only 20 publications on tire pyrolysis. In addition, a new search was carried out in the Scopus platform, and the number of publications found was 18. The publications by Brazil re­ searchers until now have not reported the potential of TPO production since their focus was different. However, it is relevant to specify this potential, since Brazil is one of the 10 countries with the largest number of waste tires generated per year [30]. Furthermore, analysis of the properties of the TPO involved in the atomization phenomenon is important, because this enables predicting the quality of the fuel spray and the physical homogeneity of the TPO produced in different parts of the world. To contribute to the promotion of fuel production from waste, this work presents detailed information on the amount of feedstock available and the estimated potential production of TPO in Brazil per year. In addition, evaluation of the stability of TPO and its ability to blend with diesel oil (DO) is performed.

data declared by the manufacturers and importers of new tires and waste tire collection companies in Brazil, in order to comply with the pro­ visions of CONAMA (National Environmental Council) Resolution 416 [31]. The data provided in IBAMA’s annual reports [32–39] were organized into three categories, as detailed below. 2.1.1. Tires manufactured and imported in Brazil The types of tires sold in Brazil are for trucks, vans, passenger cars, motorcycles, agricultural implements, industrial machines, airplanes and off-road vehicles (ORV). Members of the National Tire Industry Association (ANIP) from 2006 to 2016 manufactured about 695 million tires marketed in Brazil. Fig. 1 shows the number of tires manufactured per year and the numerical percentage of each type of tire, from 2006 to 2016, according to the ANIP [40]. As can be seen in Fig. 1, passenger car tires are those mainly man­ ufactured in Brazil, followed by motorcycle, van and truck tires. In 2016, these tires accounted for 98.7% of the 67.87 million tires produced. On the other hand, airplane tires represent the lowest percentage of tires manufactured in Brazil, less than 0.1%. Despite the variety of tires made in Brazil, the chemical composition of each type is similar, so that the liquid fuel produced from the pyrolysis of different types of tires does not present significant differences, as shown in Table 1. Table 1 shows the great similarity between the elemental composi­ tion and the physicochemical properties of liquid fuel obtained from tires of different types and countries. However, the TPO yield is greater for truck tires, since they contain a greater percentage of volatiles in comparison of motorcycle and passenger car tires. Some researchers have reported that for motorcycle and passenger car tires, the mass percentage of volatiles is 57.5% [43] and 58.2% [44], respectively, while truck tires contain between 65 and 66% [41,44]. Another source of feedstock for the production of TPO is the waste generated by the imported tires marketed in Brazil. In 2017, import participation in the tire replacement market was 26.9% compared to 73.1% produced domestically [39]. The mass of tires sold in Brazil (manufactured and imported) from 2009 to 2010 to 2017 [32–39] is presented in Fig. 2. Fig. 2 shows that the mass of tires produced locally and imported between 2011 and 2017 was uniform, since these values ranged from only 1.14 to 1.37 million tons. The 2009–2010 category took into ac­ count the tires imported and manufactured in 2010 and the last quarter of 2009, since the 2009 and 2010 data are not available separately.

2. Materials and methods The aims of this work were achieved through two evaluations: quantitative and qualitative. The quantitative assessment included estimation of the feedstock available and the potential for TPO pro­ duction in Brazil. The qualitative assessment involved measurements of the calorific value, specific mass, kinematic viscosity and surface tension (main atomization properties) of the TPO and DO produced in Brazil. In addition, the measured values of the TPO and DO properties were used to determine the expected droplet size of the fuel spray generated from a twin fluid atomizer.

2.1.2. Tires exported and sent to vehicle assemblers In Brazil, the amount of tires exported and sent to vehicle assemblers is in the range of 400 thousand to 590 thousand tons per year. Detailed information was collected from the annual statistical reports published by IBAMA between 2009 and 2010 to 2017 [32–39], Fig. 3. In the 2009–2010 and 2011 IBAMA statistical reports, the amounts of tires exported tires and sent to assemblers were not presented sepa­ rately. From the data in the subsequent reports, the percentages by weight of tires exported and those sent assemblers are presented in Fig. 3. It shows that the number of tires sent to assemblers began to decrease in 2013. This decrease is associated with the reduction in vehicle sales in Brazil after 2013. According to the Automotive Vehicles Distribution National Federation [45], the sale of motor vehicles (au­ tomobiles, light commercial vehicles, trucks, buses, motorcycles, and implements) in 2013 fell 2.3%, and the decline continued, reaching 20.3% in 2016 in comparison with 2012.

2.1. Feedstock available for the production of TPO The available feedstock (F) for the production of pyrolysis oil consists of the tires discarded as waste each year in a country. Waste tires generated in Brazil have two origins: tires manufactured in the country (M) and imported tires (I). However, some of the tires manufactured and imported are exported (E) or sent to vehicle assemblers (A), so that the net amount of tires in Brazil that will be discarded as waste can be calculated according to equation (1). F¼MþI

ðE þ AÞ

(1)

2.1.3. Destinations of waste tires collected in Brazil The Brazilian government has created legal mechanisms that allow the effective collection of waste tires distributed in the country. CON­ AMA Resolution 416 [31] obliges manufacturers and importers to give adequate destination to the same amount of tires that they sell (ratio 1: 1). Manufacturers and importers almost fully meet the target set by the resolution [31], reaching collection of up to 99.6% by weight of tires

Since 2011, the Brazilian Institute of Environment and Renewable Natural Resources (IBAMA) has been publishing annual reports based on 1 The key words used in the research were: Tire pyrolysis, Brazil, feedstock, tire pyrolysis oil, potential production.

2

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Fig. 1. Tires manufactured per year and numerical percentage of each type of tire from 2006 to 2016. Adapted from ANIP [40].

3

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devulcanization), shale processing and pyrolysis [39]. The technologies used in Brazil for environmentally correct destination of waste tires are presented in Fig. 4, along with the percentages of tires processed by each technology from 2009 to 2010 to 2017 [32–39]. According to Fig. 4, the technologies most used in Brazil to process waste tires are coprocessing, granulation and lamination, which consume 98% of the waste tires collected. On the other hand, only about 2% goes for regeneration, shale processing and pyrolysis. Pyrolysis has been considered a technology for processing waste tires in Brazil only since 2012 [34]. In that year, only 336 tons of waste tires were sent for pyrolysis, which represented 0.07% of the total tires collected. In 2017, the mass percentage for pyrolysis technology increased to 2.26%, equivalent to 13.21 thousand tons, still an insig­ nificant amount in relation to those treated by other technologies. The largest percentage of waste tires collected is destined for coprocessing technology, about 55%, but this has the disadvantage of using the waste tires as fuel without changing the composition. A typical tire’s elemental composition is between 1.2% and 2.5% by mass of sulfur [5,13,41,46], which can be converted into SOx during burning. How­ ever, in pyrolysis, the sulfur is distributed among its products: liquid, gas and solid. In order to know the distribution of the tire sulfur in each of the pyrolysis products, experimental data were collected and, in some cases, an estimate was made using the principle of mass conservation and the data found in the literature on the composition and yield of each pyrolysis product. Table 2 summarizes the articles and estimated sulfur distribution in each tire pyrolysis product. Table 2 shows that most of the sulfur in tires goes to make solid products, followed by TPO and finally pyrolysis gas. The average per­ centages of sulfur captured, according to the data in Table 2, in solid, liquid and gas form from tire pyrolysis were 63.3%, 24.8%, and 11.9%, respectively. Therefore, during the burning of an equal mass of tires and TPO, assuming that all the sulfur is transformed only to SO2, the amount of SO2 formed in the case of TPO would be only 24.8% of the mass of SO2 formed in the combustion of the tires. This advantage makes TPO a less polluting fuel than the untreated tires, so the pyrolysis technology can be classified as environmentally superior to coprocessing. However, the two major producers of waste tires in Latin America, that is, Brazil and Mexico, allocate about 50% of the total as fuel for cement kiln [30,39].

Table 1 Elemental composition and properties of TPO produced from different types of tires. Features

[41]

[42]

[43]

[44]

[44]

Tire

Truck

Car

Motorcycle

Truck

Origin

South African Conical spouted bed 475

Brazil

India

Passenger car Turkey

Fixed batch

Fixed-bed fire tube heating

Fixed Bed

Fixed bed

450

475

650

650

58.2

45.0

49.0

48.4

56

n.i

931.3

943

913

n.i

5.95

a

42.7

42.0

86.0

Reactor Tpyrolisis (oC) TPO yield (wt.%) Density (kg/m3) Viscosity (cSt) HHV (MJ/ kg) Carbon (wt. %) Hydrogen (wt.%) Nitrogen (wt.%) Sulfur (wt. %) Oxygen (wt. %)

957

4.62

3.85c

42.0

41.6

42.4

85.71

85.86

87.57

86.47

10.8

10.01

9.15

10.35

11.73

0.3

0.32

0.65

<1

<1

1.2

n.i

1.25

1.35

0.83

1.7

n.i

2.87

n.i

n.i

4.75

b

c

Turkey

n.i: not informed; Tpyrolisis: Pyrolisis temperature; HHV: Higher Heating Value; a: 20 � C; b: 30 � C; c: 40 � C. Adapted from Refs. [41–44].

sold according to 2018 IBAMA statistical report [39]. The management system of waste tires defined by CONAMA resolution 416 is called Extended Producer Responsibility (EPR), which is one of the three main systems considered in the world (EPR, tax system and free market). Waste tires collected in Brazil are mainly used for: coprocessing (fuel in clinker kilns), lamination (manufacture of rubber articles), granula­ tion (manufacture of ground rubber), regeneration of rubber (rubber

Fig. 2. Mass of tires manufactured and imported in Brazil from 2009 to 2017. Adapted from IBAMA [32–39]. 4

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Fig. 3. Mass of tires exported and sent to vehicle assemblers in Brazil from 2009 to 2017. Adapted from IBAMA [32–39].

2.2. Potential production of TPO in Brazil

reserve to production ratio (R/P). This ratio represents the time at which a given reserve would be exhausted if its production remained constant over time [61]. Fig. 5 shows the evolution of the R/P ratio of Brazilian petroleum in the last 20 years [62–79]. According to Fig. 5, the R/P of petroleum in Brazil has undergone a significant drop in the last 20 years, from 23.2 to 13.4 years. In addition, the trend of the R/P is naturally decreasing since petroleum is an exhaustible resource. Although new petroleum reserves have been discovered (pre-salt petroleum), the downward trend of R/P will continue over time, so new alternative sources should be promoted, such as TPO production.

In Brazil, about 500 thousand tons of waste tires are collected per year by manufacturers [39]. The effectiveness of this effort has been made possible by the creation of the industry organization RECICLANIP in 2007. In 2018, there were 1053 collection points distributed throughout the country operated by the organization [55]. However, recycling technologies such as pyrolysis have not been adequately pro­ moted in Brazil, see Fig. 4. Various studies have shown it is possible to recover a significant percentage of TPO from a tire. Table 3 presents a summary of data published on the product yields from tire pyrolysis under different processing conditions. Table 3 shows that the TPO yield obtained from the pyrolysis of tires with different reactors and temperatures (between 350 and 800 � C) is in the range of 25.3–62.8%. The mean of the values shown in Table 3 can be considered representative of the product yields from tire pyrolysis. Therefore, 44.1% was considered as an unbiased value of TPO yield, according to the statistical definition of sample mean. The potential mass of TPO can be calculated once the mass of available feedstock (waste tires) is determined. Then the potential mass of TPO can be expressed in volumetric units if a representative density value is considered for the TPO. Table 4 presents values of TPO density at 20 � C published by some researchers. The data in Table 4 were used as representative to determine the TPO density at 20 � C. Thus, the sample mean of the values in Table 4, that is, 921.2 kg/m3, was assumed to be the density of the TPO. In order to determine the volumetric potential of TPO (PV), equation (2) was used, which was constructed from equation (1) with the inclusion of some multiplicative factors. PV ¼ kw ⋅ ½M þ I

ðE þ AÞ� ⋅ xTPO ⋅ρTPO

2.3. Tire pyrolysis oil produced in Brazil TPO has similar characteristics to fuel oil (FO), used for the gener­ ation of thermal energy in furnaces and boilers [80]. Brazilian FOs originate from petroleum refining and shale pyrolysis. These FOs are classified, according to the National Agency of Petroleum, Natural Gas and Biofuels (ANP) Resolution 3 [81] as low sulfur content and low viscosity (OCB1), low sulfur content and high viscosity (OCB2), high sulfur content and low viscosity (OCA1) or high sulfur content and high viscosity (OCA2). In turn, ANP Resolution 48 [82] also establishes specifications for FOs intended to replace natural gas in turbines for power generation. For comparative purposes, Table 5 presents specifi­ cations of the types of FOs produced and sold in Brazil (types E and G) along with some properties of TPO reported in the literature. According to Table 5, TPO has similar sulfur content and upper heating value and better kinematic viscosity than the FO produced in Brazil. The low TPO viscosity allows saving energy when passing the fuel through injection and transport lines because it requires lower pressure compared to that required by a typical FO, with viscosity of 960 cSt. On the other hand, TPO’s flash point varies between 13.5 � C and 61 � C. This variability is associated with the content of flammable volatiles (boiling temperatures lower than 93 � C), which are 10% of the volume of TPO [14]. These volatile components evaporate when the TPO is stored incorrectly, causing the initial flash point to increase. The data presented in Table 5 on the TPO produced in different parts of the world and in different years shows the quality and homogeneity of

(2)

The multiplicative factors included in equation (1) are TPO yield (xTPO ), TPO density at 20 � C (ρTPO ) and the new tire wear factor (kw ). The assumed value for kw was 0.7, because CONAMA Resolution 416 [31] defines a 30% reduction in mass of a new tire when it has completed its useful life. One of the main contributions to promote the production of TPO is the preservation of non-renewable resources, and the increase of the 5

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Fig. 4. Technologies used in Brazil for environmentally correct destination of waste tires and percentages of tires processed by each technology. Adapted from IBAMA [32–39].

TPO. However, characterization of the TPO produced in Brazil was carried out to verify if its properties are comparable with those of the TPOs produced in other parts of the world. In this work, the TPO was obtained from the Brazilian cement company Polimix, which has the capacity to recycle 30 thousand tons of waste tires per year through the continuous pyrolysis process for the production of carbon black, oil (TPO) and steel [88]. Polimix made two donations of TPO: crude (CRTPO) and centrifuged (CETPO), which were characterized. After­ ward, CETPO was exposed to the environment for three and twenty days to simulate storage conditions, which were represented by CETPO1 and CETPO2, respectively. In addition, blends were formed between TPO and diesel oil (DO), which were also characterized. DO was purchased from a Petrobras service station as S10 diesel, whose technical specifi­ cations are available at the Petrobras website [89]. The measured properties of the four samples were the higher (or upper) heating value (HHV), kinematic viscosity, density and surface tension. The devices used to measure these properties were: IKA C1 colorimeter, Lauda Proline PV15 viscometer, Rudolph Research Analytical DDM 2911 dig­ ital densimeter and Traube stalagmometer. The measured properties of the TPO and DO samples were used to determine the expected mass median diameter (MMD) of the spray generated by a twin-fluid atomizer (air-fuel). The equation used to

determine the expected MMD was the dimensionally correct correlation of Wigg [90], equation (3), which provided satisfactory predictions for Mullinger and Chigier [91] in evaluating the effect of operational con­ ditions on the performance of Y-jet atomizers. � �0:5 200⋅νf 0:5 ⋅ðQ_ th =LHVÞ0:1 ⋅ 1 þ m_ f m_ a ⋅h0:1 ⋅τf 0:2 MMD ¼ (3) ρa 0:3 ⋅Ua Where νf is the fuel kinematic viscosity, Q_ th is the atomizer thermal power, LHV is the lower heating value of fuel, m_ f =m_ a is the fuel-air mass ratio, h is the radius of the atomizer mixing chamber, τf is the fuel surface tension, ρa is the air density, and Ua is the air velocity. According to Mullinger and Chigier [91], Ua may normally be assumed to be the critical velocity of the atomizing fluid and ρa the atomizing fluid supply density. To calculate Ua , the air flow was assumed to be unidimensional and isentropic, so the compressible flow theory was applied. Addition­ ally, the value of the LHV was assumed equal to the HHV in order to simplify the calculation. The atomizer considered to apply equation (3) was the Y-jet type (twin-fluid), whose internal geometric characteristics are presented in Fig. 6. The geometric dimensions shown in Fig. 6 were determined for a 50 kW thermal power atomizer, which operates with air as auxiliary fluid. 6

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Table 2 Sulfur distribution in tire pyrolysis products.

Table 3 Product yields from tire pyrolysis under different processing conditions.

Reference

Tpyolysis [oC]

Liquid [wt.%]

Solid [wt.%]

Gas [wt.%]

[5] [5] [5] [7] a [47] a [48] [48] [48] [48] [48] [49] [49] [49] [50] a [51] a [52] a [53] [54] [54] [54] [54]

425 475 575 600 550 600 650 700 750 800 350 450 550 550 600 600 500 400 500 550 700

35.0 34.1 33.2 23.3 26.2 20.1 15.4 14.2 12.8 12.3 21.7 25.7 33.8 37.2 36.5 22.6 20.0 22.0 25.2 22.6 27.7

58.7 58.5 63.0 67.7 66.7 68.6 68.1 67.1 67.5 61.9 75.0 60.0 51.1 61.6 53.4 52.4 51.0 66.7 70.4 69.2 71.0

6.3 7.4 3.8 9.0 7.1 11.3 16.5 18.7 19.7 25.8 3.3 14.3 15.1 1.2 10.1 25.0 29.0 11.3 4.4 8.2 1.3

Reference

Reactor

Tpyrolysis [oC]

Liquid [wt.%]

Solid [wt.%]

Gas [wt.%]

[4] [5]

Fixed bed Conical spouted bed Conical spouted bed Conical spouted bed Fluidized bed Fluidized bed Fluidized bed Fluidized bed Moving bed (screw) Moving bed (screw) Moving bed (screw) Static stirred batch Static stirred batch Static stirred batch Static stirred batch Fixed bed Continuous auger Continuous Rotary kiln Continuous Rotary kiln Continuous Rotary kiln Continuous Rotary kiln Continuous Rotary kiln Autoclave Autoclave Autoclave Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed Fixed bed

400 425

38.8 58.5

34.0 37.9

27.2 3.6

475

58.4

35.9

5.7

575

53.9

35.9

10.2

400 475 550 600 600

44.0 40.6 29.3 25.3 41.5

33.5 34.5 40.5 28.7 40.6

22.5 24.9 30.2 46.0 17.9

700

31.3

39.0

29.7

800

27.5

41.0

31.5

430

43.3

48.7

8.0

450

49.0

44.0

7.0

470

53.5

40.0

6.5

500

55.5

40.0

4.5

500 550

40.0 42.6

36.0 40.5

24.0 16.9

450

43.0

43.9

13.1

500

45.1

41.3

13.6

550

44.6

39.9

15.5

600

42.7

39.3

18.0

650

42.9

38.8

18.3

500 600 700 450 500 550 600 650 700 550 500 350 400 450

38.0 38.2 38.5 37.7 40.2 39.2 38.7 38.5 39.7 38.0 58.8 53.2 62.8 57.2

44.8 44.2 43.7 51.9 47.9 47.1 45.4 43.6 41.6 33.0 38.3 43.7 26.0 25.5

17.2 17.5 17.8 10.4 11.9 13.7 15.9 17.9 18.7 29.0 2.9 3.1 11.2 17.3

[5] [5] [6] [6] [6] [6] [7] [7] [7] [12] [12]

a

Value calculated from literature data. Adapted from Refs. [5,7,47–54].

[12] [12]

The method followed to determine the geometry of the Y-jet atomizer was that presented by Mulinger and Chigier [91], taking into account an ideal gas behavior for air with stagnation properties (temperature and pressure) of 25 � C and 500 kPa. Moreover, the MMD was evaluated as a function of the air-to-fuel mass ratio in the range of 0.02–0.15, as rec­ ommended by Lacava [92] in the design of Y-jet atomizers.

[13] [47] [50] [50] [50]

3. Results and discussion

[50]

3.1. Feedstock available in Brazil

[50]

The estimated values of the amount of feedstock available in Brazil for the production of TPO per year were obtained by inserting the data of Figs. 2 and 3 in equation (1), taking into account the multiplicative factor of 0.7 corresponding to new tire wear. However, the estimated amounts of feedstock do not represent the mass of waste tires collected per year in Brazil (Fig. 4). Fig. 6 shows the amount of feedstock available in Brazil and the mass percentage collected of waste tires from 2009 to 2017. As can be seen in Fig. 7, there is a large amount of feedstock in Brazil for the production of TPO, which is in the range of 480 thousand to 588 thousand tons per year. Although more than 84% of this quantity is collected per year, this still leaves almost 200 thousand tons not collected from 2009 to 2017, causing substantial environmental liabilities.

[52] [52] [52] [56] [56] [56] [56] [56] [56] [57] [58] [59] [59] [59]

Tpyrolysis: Pyrolysis temperature. Adapted from Refs. [4–7,12,13,47,50,52,56–59].

3.2. Potential production of TPO in Brazil

Table 4 TPO density at 20 � C reported in the literature.

Based on equation (2), the previous assumptions of TPO yield, TPO density at 20 � C and the data in Fig. 7, the potential volumetric amount of TPO (considering 100% collection) per year in Brazil was estimated. The results obtained for 2010 to 2017 are presented in Fig. 8 along with the total volumetric amount of shale fuel oil produced in Brazil in the last 20 years [62–79]. Fig. 8 shows the quantitative importance of TPO, since amounts comparable to shale oil could be produced in Brazil. The potential production of TPO is in the range of 230 thousand to 280 thousand m3 a year. Meanwhile, the volume of shale fuel oil produced in Brazil be­ tween 2010 and 2017 was in the range of 213 thousand to 346 thousand m3. On the other hand, a quantitative comparison is presented in Fig. 9

Reference

Density at 20 � C [kg/m3]

[8] [14] [19] [21] [22] [42] [43] [46] [50] [60]

900.0 875.0 910.0 920.0 913.0 931.3 957.0 912.3 962.0 931.3

Adapted from Refs. [8,14,19,21,22,42,43,46,50,60].

7

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between the potential amount of TPO and FO produced in Brazil [79] due to the great similarity between those fuels, as presented in Table 5. Furthermore, Fig. 9 presents the comparison between the potential amount of TPO and the onshore petroleum extracted in Brazil [79]. This comparison was made due to the possible use of TPO as feedstock for the production of gasoline and diesel oil, as reported by some authors [28, 29]. As can be seen in Fig. 9, the potential TPO represents about 2% of the total volume of fuel oil produced in Brazil, and in the case of onshore petroleum represents above 2.2%. These percentages are small, but they are significant because in 2017, 11.7 million m3 of FO was produced and 7.4 million m3 of onshore petroleum was extracted [79]. FO in 2017 represented 11.4% of the total production of energy derivatives, and in that year the energy derivatives produced in the refineries reached 96.5 million m3 [79]. Furthermore, potential output of TPO in Brazil is comparable to total petroleum production (onshore and offshore) in some of the 11 states with the highest production in Brazil, such as Maranh~ ao, Cear� a and Alagoas, which produced 2, 319 and 189 thousand m3 in 2017, respectively [79].

Fig. 5. Evolution of the R/P ratio of Brazilian petroleum from 1997 to 2017. Adapted from ANP [62–79].

3.3. Brazil and other countries

Table 5 Technical specifications of the types of FO produced and sold in Brazil and some properties of TPO reported in the literature. Type

Kinematic viscosity [cSt]

ANP resolution no 3 [81] OCB1 620e OCB2 960e OCA1 620e OCA2 960e ANP resolution no 48 [82] OCTE 1.60–6.00c TPO reported in literature [4] 0.95d [5] n.i. [8] 2.81c [10] 2.10–3.69c [14] 1.70c [19] 2.38e [22] 3.35a [23] 5.06c [29] 3.21c [43] 4.75b [44] 3.85c [47] 2.87c [49] n.i. [50] 1.63–3.66d [51] n.i. [52] n.i. [56] 3.80c [80] 9.7d [83] 1.17n.i. [84] 6.61c [85] 3.77d Marketed Shale oil Tipo E 48.00e max. [86] Tipo E 48.00e [87] Tipo G 5.00e max. [86] Tipo G 7.00e [87]

Sulfur [wt. %]

Flash point [oC]

HHV [MJ/ kg]

1.00 1.00 2.00 2.00

66.00 66.00 66.00 66.00

40.14 40.14 40.14 40.14

1.00

38.00

40.14

1.07 1.20–1.30 0.60 1.23–1.76 0.59 1.45 0.95 1.13 1.42 1.25 0.83 0.80 1.30–1.60 0.97–1.54 1.99–2.40 1.00–1.40 0.91 0.80 0.80 1.37 0.72

61.00 n.i. 20.00 n.i. <30.00 20.00 49.00 42.5 28.10 <32.00 <30.00 n.i. n.i. 13.50–30.00 n.i. n.i. 50.00 28.00 n.i. n.i. 43.00

42.61 42.5–42.80 43.27 38.93–42.05 43.80 42.10 38.10 39.90f 41.00 42.00 42.40 42.45 37.43–40.78 41.00–41.90f 42.48–44.81 42.10–43.20 43.34 43.70 42.00 41.31 38.00

2.50 max.

66.00 min.

42.57

1.00 max.

66.00 min.

42.57

2.50 max.

66.00 min.

42.90

1.00 max.

66.00 min.

42.90

The amount of waste tires generated by Brazil in 2017 [39] was compared to those of countries that cover 89% of vehicles in the world [30], as shown in Fig. 10. In addition, Fig. 10 shows the main ways to recover waste tires and the different management systems applied by those countries. As shown in Fig. 10, China, United States, and India are the countries that generate the largest amount of waste tires per year in the world, which together contribute almost 65% of the total. However, Brazil is among the ten countries that generate the largest amount of waste tires per year and ranks second in the Americas, surpassed only by United States. In spite of China, United States, India, Japan, and Brazil being the countries that generate the largest amount of waste tires, they have re­ covery rates of over 85%. This fact may be associated with the applied management system, where EPR and free-market systems are the most popular, as shown in the figure, and through which the highest recovery rates have been achieved. In Europe, 66% of countries apply an EPR system, 28% a free-market system and only Denmark, Slovakia, and Croatia apply a tax system (government responsibility, financed through a tax) [30,93]. Brazil applies an EPR system and, in 2017, achieved a 99.5% re­ covery rate [39], whereas countries such as India and United States, which have a free market system, achieved recovery rates of 98 and 87%, respectively. On the other hand, Canada achieved a 111% recovery rate by applying a hybrid system based on basic requirements at the federal level, recycling programs administered by non-profit organiza­ tions and fee collected in new tires purchased [30]. The global scenario, Fig. 10, shows that the current main routes for recycling waste tires are material (47%) and energy (20%) recovery, while an important 30% corresponds to waste tires not recovered (sent to landfills, stockpiled or unknown destination). In the Americas, about 41% of waste tires are recovered as alternative fuels, mainly for cement kilns. The countries in the Americas with the highest percentages of waste tires destined for cement kilns are Brazil and Mexico with 47% [39] and 52% [30], respectively, whereas the United States allocates only 19% [30]. On the other hand, countries such as Thailand, Indonesia, China, and Malaysia have placed emphasis on alternative recycling technologies such as pyrolysis, each of them allocating 30, 35, 11 e 10% [30], respectively, which are larger than the percentage allocated by Brazil (2%) [39].

n.i.: not informed. max.: maximum limit; min.: minimum limit. a 20 � C. b 30 � C. c 40 � C. d 50 � C. e 60 � C. f lower. Adapted from Refs. [4,5,8,10,14,19,22,23,29,43,44,47,49–52,56,80–87].

3.4. Properties of TPO produced in Brazil The properties of the four TPO samples (CRTPO, CETPO, CETPO1, CETPO2) were compared to evaluate the effect of centrifugation and 8

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Fig. 6. Internal geometry dimensions of Y-jet atomizer. Gamboa et al. (2019)

Fig. 7. Feedstock available in Brazil and mass percentage collected of waste tires from 2009 to 2017. Gamboa et al. (2019)

exposure to the environment (storage conditions). Furthermore, the four TPO samples were blended with DO to evaluate the occurrence of syn­ ergistic and antagonistic effects.

properties of the four TPO samples, along with the properties of the DO and data collected from the literature on the properties of TPO. Table 6 shows that the HHV of CETPO did not change significantly with exposure to the environment, even for a time of twenty days. Moreover, the energy quality of the TPO improved slightly when it is centrifuged. The HHV taken as representative of the literature corre­ sponds to the mean of the TPOs presented in Table 5. The HHV of 41.82 MJ/kg, with standard deviation of 1.77 MJ/kg, shows the homogeneity

3.4.1. Influence of exposure of TPO to the environment The exposure times of three and twenty days were chosen because for times shorter than three days and longer than twenty days, no significant changes in the properties of CETPO were observed. Table 6 shows the 9

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Fig. 8. Potential volumetric amount of TPO and volumetric amount of shale fuel oil produced in Brazil. Gamboa et al. (2019) and ANP [62–79].

Fig. 9. Percentage representation of potential amount of TPO in relation to fuel oil and onshore petroleum produced in Brazil. Gamboa et al. (2019)

of the TPO produced in different countries, including Brazil. Table 6 also shows the high HHV of the four TPO samples, which are comparable to that of DO (45.30 MJ/kg). Conversely, the exposure to the environment of the TPO slightly changed its density. The exposure of CETPO to the environment for three days increased its specific mass by 5.1%, while after twenty days of exposure the density increased by 5.6%. These increases directly affected the API gravity of CETPO. Before the CETPO was exposed, it had a value of 22.3� API (medium oil), and that value decreased to 14.9� API (heavy oil) and 14.1� API (heavy oil) after exposure of three (CETPO1) and twenty (CETPO2) days, respectively. In contrast, the API gravity of DO was 34.4� , which indicates the higher concentration of paraffinic components in that fuel. In addition, the similarity between the density

measurements of the four TPO samples and the reported data from the literature show the physical homogeneity of the tire oil produced in different parts of the world under different pyrolysis conditions. The property of CETPO most affected by exposure was kinematic viscosity. It increased approximately fourfold when the exposure time was twenty days. However, the viscosity value of CETPO2 was much lower than the values required by ANP Resolution 3 [81] for FO, whose values are in the range of 620–960 cSt. The value of 3.65 cSt for the TPO (literature) corresponds to the mean of the values presented in Table 5 for the kinematic viscosity at 40 � C of the TPO. The standard deviation of 1.44 cSt shows the great physical similarity of TPOs produced in different parts of the world, including Brazil. There are few reports in the literature of TPO surface tension, but it is 10

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Fig. 10. Waste tire generation, management systems and recovery routes by country. Adapted from Refs. [30,39,93].

values of CRTPO, CETPO, CETPO1, CETPO2 and DO sprays generated with the previously described Y-jet atomizer, Fig. 6, operating at the airto-fuel mass ratio range of 0.02–0.15, are shown in Fig. 11. Fig. 11 shows that the atomization of CETPO2 has lower quality than CRTPO, CETPO, and CETPO1. The expected value of the MMD for CETPO2 was 1.6 times greater than that of the DO, whereas for CETPO it was 1.1 times. Therefore, the atomization quality is only slightly affected by exposure to the environment, but the atomization quality of the TPO is comparable to that of the DO. Furthermore, a suitable and stable MMD for TPO can be obtained if the air-to-fuel mass ratio is greater than 0.05, since MMD below 60 μm can be achieved.

Table 6 Atomization properties of CRTPO, CETPO, CETPO1, CETPO2 and DO. Sample

HHV [MJ/ kg]

Densitya [kg/ m3]

Viscosityb [cSt]

Surface tensionc [mN/m]

CRTPO

42.28 � 0.12 42.52 � 0.15 41.88 � 0.08 41.94 � 0.15 41.82 � 1.77 45.30 � 0.08

936.68 � 0.06

2.87 � 0.01

29.35 � 0.66

916.71 � 0.06

2.49 � 0.01

29.76 � 0.68

963.44 � 0.06

2.26 � 0.01

30.33 � 0.66

968.39 � 0.06

8.28 � 0.02

29.41 � 0.66

921.19 � 25.84 850.04 � 0.06

3.65 � 1.44

29.43 � 0.23

3.94 � 0.04

28.10 � 0.66

CETPO CETPO1 CETPO2 Literature DO

3.4.2. Blends of TPO and DO The TPO and DO mixtures were prepared by mechanical stirring. Initially, DO was blended with CETPO samples exposed to the envi­ ronment (CETPO1 and CETPO2) and subsequently with CETPO without exposure. In the first blend, the instant formation of a carbonaceous solid residue in the bottom of the vessel was observed. In the second blend, those carbonaceous residues only appeared after 24 h and were most evident for volumetric percentages of TPO in the blend above 20%. A photograph of the prepared blends and the formation of carbonaceous residues is shown in Fig. 12. The formation of these solid residues comes from the asphaltenes present in the TPO, which represent about 4.8% by mass, as reported by �kov� Bi�ca a and Straka [16]. Asphaltene deposits are often observed in the petroleum industry, where they are considered undesirable. Asphaltenes are present in crude oil in the form of colloidally dispersed particles and are lyophobic relative to low molecular weight paraffinic hydrocarbons and lyophilic to aromatics and resins [95]. The change in concentrations of alkanes in the petroleum [96] or the mixture of petroleums having different chemical nature [97] can cause precipitation of asphaltenes. Thus, asphaltenes are kept in the oil in a delicate balance, whose perturbation by the addition of saturates or the removal of aromatics can lead to the formation of asphaltene deposits [97]. In the case of CETPO, CETPO1 and CETPO2, exposure modified the chemical composition. The CETPO before exposure to the environment had gravity of 22.3� API, which initially classified it as medium oil. After

a

20 � C. 40 � C. c 23 � C. Gamboa et al. (2019) b

a relevant property for the atomization of a fuel. The value presented in Table 6 as based on data from the literature corresponds to the value reported by Chumpitaz [94], and it is very close to the measured surface tension for TPO and DO. Table 6 shows that the exposure of the CETPO to the environment did not significantly modify its surface tension, whereas the numerical difference of surface tension between the different TPO samples may be associated with the random error of the measurements. The values of the main atomization properties for the four TPO samples indicated strong physical similarity with the DO. However, more information is required to evaluate the atomization quality of the TPO samples, so the expected MMD, calculated from equation (3), was used. The kinematic viscosity at 25 � C of CRTPO, CETPO, CETPO1, CETPO2, and DO were required, since the Y-jet atomizer was considered to be operating at 25 � C. The kinematic viscosity values at 25 � C of CRTPO, CETPO, CETPO1, CETPO2, and DO were 4.04 cSt, 3.39 cSt, 3.78 cSt, 14.45 cSt, and 5.93 cSt, respectively. The expected MMD 11

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Fig. 11. Expected MMD values of CRTPO, CETPO, CETPO1, CETPO2 and DO sprays using a Y-jet atomizer of 50 kW. Gamboa et al. (2019)

Fig. 12. TPO-DO blends and formation of carbonaceous residues. Gamboa et al. (2019)

exposure, the CETPO sample was classified as heavy oil, because its API gravity was below 22� . The low API gravity values of 14.9� and 14.1� for CETPO1 and CEOTPO2, respectively, show the higher presence of aro­ matic hydrocarbons (higher density) in relation to the CETPO. On the other hand, the API gravity of the diesel used was 34.4� , indicating its high paraffin content. Therefore, the formation of asphaltene deposits in the DO and TPO blend will be greater as the API gravity of TPO becomes lower. To avoid the instantaneous formation of asphaltenes when blending

DO and TPO, blends between CETPO and DO were prepared. Never­ theless, blends of CETPO and DO with volumetric percentages of TPO above 20% still presented formation of asphaltenes after 24 h. CETPO and DO blends were characterized to evaluate the presence of syner­ gistic or antagonistic effects before the formation of asphaltene deposits. The blends were represented by the percentage of CETPO in the blend as 10TPO, 20TPO, 30TPO, 40TPO, and 50TPO. The higher heating value (HHV), specific mass (ρ), kinematic viscosity (ν) and surface tension (σ ) of the blends are shown in Fig. 13, while Table 7 reports the correlations 12

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Fig. 13. (a) Higher heating value, (b) density, (c) kinematic viscosity and (d) surface tension of TPO-DO blends. Gamboa et al. (2019)

country per year. The estimated potential amount of TPO was similar to the amount of shale oil currently produced in Brazil. In addition, the potential TPO represented around 2% by volume of onshore petroleum and fuel oil produced in Brazil for both cases. Although the potential TPO represents a significant amount in the volume of fuels produced in Brazil, only 2% of collected waste tires are allocated for processing by pyrolysis. The properties of TPO produced in Brazil showed homogeneity in relation to the TPOs produced in other countries. The advantages of TPO in comparison to fuel oils produced and sold in Brazil were also evalu­ ated. The viscosity of the TPO was considerably lower than the FOs produced in Brazil, which have values up to 960 cSt. The physical similarity between TPO and DO showed that good atomization can be achieved with TPO using a conventional Y-jet atomizer. Furthermore, the similarity between the properties of TPOs produced from different types of tires and in different parts of the world encourages their pro­ duction, since a fuel with defined properties can be produced. Another important observation is the incompatibility between TPO and DO, which form organic deposits when they are blended. The deposition of organic compounds was most notable when DO was blended with highly aromatic TPO. Even with TPO stored correctly, the appearance of organic deposits was observed when the percentage of TPO in the blend exceeded 20%. An in-depth study of the correct volumetric percentages in TPO-DO blends should be performed because they are the object of different studies for application in diesel engines. However, the recommendation extends to all types of pyrolysis oils, because their chemical composition depends on the pyrolyzed material, and incompatibility between them and traditional fuels can happen, preventing their use in blends.

Table 7 Correlations obtained to HHV, density, kinematic viscosity and surface tension of TPO-DO blends. Properties

Units

Polynomial adjustment

R2

Higher heating value Density

[MJ/ kg] [kg/ m3] [cSt]

45:22

0.996

[mN/ m]

28:10 þ 3:04 � 10 y2TPO

Kinematic viscosity Surface tension at 23 � C

0:03⋅yTPO 0:71⋅T

864:73 þ 0:65⋅yTPO

0.999

9:66 2:00 � 10 1 ⋅T 5:95 � 10 2 ⋅yTPO þ 1:65 � 10 3 ⋅T2 þ 8:81 � 10 4 ⋅y2TPO 2

⋅yTPO

1:38 � 10

4

⋅

0.982 0.999

yTPO : vol. % of TPO in TPO-DO blend; T: temperature at oC. Gamboa et al. (2019)

obtained from adjustment of the experimental values in Fig. 13. As can be seen in Fig. 13a and b, there was a directly proportional relationship between the volumetric percentage of TPO in the mixture and some of its properties (HHV and density). This ratio of propor­ tionality shows the absence of synergistic or antagonistic effects in the blend of DO and TPO, before formation of asphaltene deposits. On the other hand, the kinematic viscosity and surface tension of the blend were adjusted by a second-degree polynomial. The correlations con­ structed showed a high degree of fit, since for each property the coef­ ficient of determination was above 0.98. All measurements presented in Fig. 13 are accompanied by their respective uncertainties evaluated with significance of 95%. In the cases of kinematic viscosity and density, the uncertainties were on the order of 0.01 cSt and 0.06 kg/m3, respectively, for which reason they are not seen in Fig. 13. The HHV, density, kinematic viscosity and surface tension of the TPO and its blend with DO showed the ease of atomization of the fuel, which can be achieved using conventional atomizers, such as twin-fluid or pressure devices.

Acknowledgments The authors are grateful to Polimix for the donated tire pyrolysis oil samples. This work was supported by the S~ ao Paulo State Research Foundation (FAPESP), process number 2016/10274-9.

4. Conclusions

Appendix A. Supplementary data

A detailed evaluation of the amount by weight of waste tires pro­ duced annually in Brazil was carried out. The data obtained were used to estimate the potential volume of TPO that can be produced in the

Supplementary data to this article can be found online at https://doi. org/10.1016/j.rser.2019.109614. 13

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