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Review

Plastic and Waste Tire Pyrolysis Focused on Hydrogen Production—A Review

by
Gaweł Sołowski
1,*,
Marwa Shalaby
2 and
Fethi Ahmet Özdemir
1
1
Department of Molecular Biology and Genetics, Faculty of Science and Art, Bingöl University, Bingöl 1200, Turkey
2
Chemical Engineering and Pilot Plant Department, Engineering Research Division, National Research Centre, 33 El Bohouth Street (Former El Tahrir Street), Giza P.O. Box 12622, Egypt
*
Author to whom correspondence should be addressed.
Hydrogen 2022, 3(4), 531-549; https://doi.org/10.3390/hydrogen3040034
Submission received: 16 October 2022 / Revised: 30 November 2022 / Accepted: 2 December 2022 / Published: 6 December 2022
(This article belongs to the Special Issue Theoretical and Practical Aspects of Hydrogen Production from Hydrocarbons)
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Abstract

:
In this review, we compare hydrogen production from waste by pyrolysis and bioprocesses. In contrast, the pyrolysis feed was limited to plastic and tire waste unlikely to be utilized by biological decomposition methods. Recent risks of pyrolysis, such as pollutant emissions during the heat decomposition of polymers, and high energy demands were described and compared to thresholds of bioprocesses such as dark fermentation. Many pyrolysis reactors have been adapted for plastic pyrolysis after successful investigation experiences involving waste tires. Pyrolysis can transform these wastes into other petroleum products for reuse or for energy carriers, such as hydrogen. Plastic and tire pyrolysis is part of an alternative synthesis method for smart polymers, including semi-conductive polymers. Pyrolysis is less expensive than gasification and requires a lower energy demand, with lower emissions of hazardous pollutants. Short-time utilization of these wastes, without the emission of metals into the environment, can be solved using pyrolysis. Plastic wastes after pyrolysis produce up to 20 times more hydrogen than dark fermentation from 1 kg of waste. The research summarizes recent achievements in plastic and tire waste pyrolysis development.

1. Introduction

Plastics and tire wastes are an enormous problem among society that leads to worldwide disasters. According to Gandhi et al. [1], 35 million tonnes of plastic waste and 1.7 million tons of waste tires [2] (a hybrid of biopolymer and plastic) are produced, together with almost 37 million tons of synthetic organic waste. According to Wang et al. [3], approximately 9.1 billion tons of plastics have been produced globally over the past 50 years. Plastic contamination is a worldwide problem and causes the destruction of islands’ economies, such as Grenada or Malta [4]. The problem, similar to pollution with waste tires [5], has been widely reviewed in different regions of the world, including Africa [6] and Asia [7].
Plastic has been replacing commonly used natural materials from the middle of the XIX century. The first polymers replaced ivory in some entertainment branches, e.g., snooker balls. These replacements prolonged the existence of elephants [8]. Then, plastic was frequently introduced into relatively new branches of life (e.g., radios, televisions and computers). The selection of plastic materials was a result of their outstanding mechanical, thermal, heat insulation and durability properties [9]. Robert Thomson invented tires in 1846. Synthetic polymers to support natural rubber were applied in 1920. The durability and complexity of plastic caused it to emerge as a problematic form of waste after its usage period [10].
Many polymers have smart properties such as semiconductivity [11], being better than inorganic ones (organic photovoltaics can absorb light of a broader spectrum than silicon). These excellent, often unique properties make them ideal for daily life, but they also create highly problematic waste after their functionality is expended. Updates of design and production require the fulfilment of the demands of everyday life and disposal after products become useless or outdated. The plastic recycling rate is still low, with only 19% of all waste being recycled in the US [12]. Plastic production has not decreased significantly, being ranked as the fastest-growing type of waste in the world [13]. Therefore, rapid methods of plastic and tire utilization need to be designed and developed in order to protect the environment from the negative impacts of this waste.
Plastic and tire wastes require recycling, and pyrolysis is a process involving the thermal transition of these materials into simpler organic compounds and hydrogen. Pyrolysis reverses earlier polymer production processes by applying heat to transform the used material into energy or chemicals. Pyrolysis features a rapid utilization rate compared to other approaches, such as fermentation or composting [14]. A comparison of tire catalytic pyrolysis summarized achievements in the area [15,16]. Pyrolysis is an industrially available method of plastic utilization, but it is also energy-consuming [17]. The method allows for the transformation of oil/carbon-originated wastes into other petrochemical materials, currently produced mainly directly from oil. If such a change was implanted widely, it would extend the depletion time of natural resources [18]. Table 1 presents the ash content after pyrolysis of the five most common types of plastic: polyethylene terephthalate (PET), high-density polyethylene (HDPE), polystyrene (PS), polypropylene (PP) and linear low polyethylene (LLDPE).
Among these five materials, the pyrolysis of HDPE produces the highest volume of ash [19,20]. Ash content allows the choice of suitable plastic waste for ash-originating material production, such as aromatic organic chemicals.
According to Zhou et al. [21], the presence of ash depends more strongly on the reactor type and type of pyrolysis. Besides catalyst residues, ash contains coke, which can provide material for some smart polymers or it can be conjugated. Microwave-assisted catalytic pyrolysis of PP pellets revealed 34% ash, while, for chips (2 mm × 3 mm × 1 mm), the ash content was only 0.1% [22]. In the case of HDPE, the ash content depended on the time period: at less than 10 min, there was no ash; increasing with prolonged streaming, at 55 min, it was up to 20%. Ash production is problematic due to the use of poisonous pyrolysis catalysts [12]. Separation techniques for catalysts and stabilizers from pyrolysis ash are necessary; otherwise, they occur in oxides and need cleaning from gaseous parts [23]. Then, such ash can be adopted as a reforming catalyst [24]. The other problem is the significant content of sulfurized organics (sulfides, aliphatic sulfur, sulfates); however, the proper pyrolysis method could form sorbents useful for capturing mercury compounds [25,26].
According to [27], PET pyrolysis features low ash content and this waste material is preferable for liquid fuel production. Pyrolysis’ profitability was analyzed in the example of hydrogen, one of the most demanded materials [28]. Hydrogen production by pyrolysis is considered in Table 2 as an inexpensive method in comparison to gasification or the use of algae. Dark fermentation is at least three times cheaper (in relation to SNG) or more so than other methods (even 10 times in the case of algae). Biofuel processes such as dark fermentation feature a low rate of production. Another disadvantage is the low variety of products besides hydrogen or methane in bioprocesses, replacing conventional methods that use raw materials for chemistry. Dark fermentation can only produce a small amount of ethylene, but there is still little knowledge about other chemicals’ production, such as benzene. Dark fermentation or biogas plants can produce methane or hydrogen [29], some salts [30] and organic acids [31], but not alkenes or alkynes, as with pyrolysis [32]. Anaerobic digestion provides methane and fertilizers [33] in biochar form [34] or by digested material compost [35,36]. In the case of the production of organic compounds of C > 2, pyrolysis is slightly cheaper than gasification, with a more extended variety of products than available bioprocesses. Microbial electrochemical cells are suitable for ammonia splitting due to their low voltage potential of only 0.06 V, in contrast to water, with a value of 1.17 V (higher by approximately 0.93 V above the MEC maximal voltage) [37]. The conversion of feed is high at 32 m3/m3 MEC d−1 [38,39]. Biological decomposition cannot utilize plastic wastes and thus cannot solve the serious problems of plastic and waste tires. The main problems of pyrolysis involve obtaining a proper catalyst optimally from waste, while biological methods have unique enzymes already existing in organisms. Catalysts can work at a wide range of temperatures, while enzymes operate in in narrow ones (usually below 55 °C), limiting their operational potential and rendering them unable to degrade polymers of high activation energy (often obtained by high temperatures). Pyrolysis decomposition is fast, allowing the desired conversion, but it is highly energy-consuming [40] in comparison to biological reactions requiring enzymes based on special conditions: they need special substrates with a particular concentration range, contrary to pyrolysis, which are sometimes light (in the case of photofermentation or the special sequential preparation of bacterial seeds) [41]. Pyrolysis has a higher conversion rate, requiring the usual changes in the catalytical layer (more than enzymes in biological cases), fulfilling the high demand for energy and for a high-strength material to construct reactors, which are more expensive than bioprocesses but require less space to obtain a similar production rate [42]. The pandemic’s demand for a rapid solution for the removal of safety protection wastes caused an increase in interest in the pyrolysis of plastic wastes [43,44,45].
Contrary to most types of utilization, pyrolysis can decompose every type of waste with hydrogen production (see Table 2). Dark fermentation can digest only natural organics, with some exceptions, such as asbestos [46] or glycol ethylene [47,48].
Table
Table 2. Costs of different hydrogen production methods [49,50].
Table 2. Costs of different hydrogen production methods [49,50].
TypeCostsRemarks
Dark FermentationFrom 0.17 $/m3 to 0.23 $/m3Cheap but low rate ability per year
Hydrogenotrophic anaerobic digestionFrom 0.16 $/m3 to 0.231 $/m3Most produced hydrogen is used for improving methane yield; the hydrogen produced has lower concentration and is more unstable than in dark fermentation
MECFrom 0.74 $/m3 to 1 $/m3Suitable for ammonia and urine wastes that need voltage low enough to split compounds without extra energy coming from fossil sources
AlgaesFrom 2.6 $/m3 to 3.68 $/m3Sensitive, large area. Expensive in comparison to other methods. By-products could be used in cosmetics
PyrolysisFrom 1.25 $/m3 to 2.2 $/m3The versatility of waste reduced emissions in comparison to gasification, possibility of production of smart polymers
Gasification1.65 $/m3Versatility of waste but high emission of toxic oxides
SNG0.67 $/m3From fossil fuels
Looking at Table 2, the differences between gasification and pyrolysis are not clearly defined. Lewandowski et al. [51,52] considered pyrolysis and gasification as one process, similar to dark fermentation and hydrogenotrophic anaerobic digestion [53,54]. The pyrolysis of plastics differs in heat demands with crystallinity. Amorphous PS has lower energy of decomposition than semicrystalline PET [55]. Major problems include metal retardants and catalyst residues from the production of plastic, which create hazardous emissions, and methods of avoidance have been described [56]. Another issue is the reactor design and modeling, with many different challenges compared to bioprocessing, as considered and described in a review. The huge activity in the pyrolysis of plastic and tires has caused the publication of many papers, requiring continuous updating through a review of achievements. The objectives of such reviews are the comparison of recent solutions that allow us to solve the problems of both types of waste more efficiently.

2. Materials and Methods

The analysis selected papers due to their results, the actual scientific interest of the chosen paper and new insights presented in the research. The articles were searched by the following queries in Scopus and Google Scholar: plastic waste pyrolysis, waste tire pyrolysis, hydrogen production from plastic wastes, hydrogen production from waste tires, contaminants from pyrolysis of plastic, contaminants from pyrolysis of waste tires, and assessment of hydrogen production from pyrolysis. The review was performed by selecting papers with data from years 1950–2022 on Scopus, focusing on years 2020–2022. During this period, 5844 papers studied plastic waste pyrolysis (487 in 2020 and 477 in 2021) and 1117 papers focused on waste tire pyrolysis (99 in 2020 and 123 in 2021); they were reviewed from September 2020 to October 2022. Both plastic and waste tire pyrolysis were the subjects of 144 papers, including 14 in 2020 and 20 in 2021. This record scientific interest in waste tire pyrolysis is progressing into a wider interest in the co-pyrolysis of plastic waste and tire pyrolysis [57]. The increase in plastic pyrolysis has been caused by a sudden increase in plastic waste connected with the COVID-19 pandemic, such as masks [58]. The review was enriched with some papers on the life cycle, renewable energy sources, circular economy and environmental production. These papers provide a general view of the problems and challenges that can be solved by the development of plastic and tire pyrolysis, sample preparation and measurement. Additionally, for the comparison of hydrogen production between dark fermentation and pyrolysis, some examples were chosen for an economic and technological comparison.

3. Results and Discussion

3.1. Review of Pollution Risk of Tire and Plastic Waste Pyrolysis

The pyrolysis method should be designed so that heavy metals and halogens can be separated from the remaining products optimally before the process as they inhibit decomposition processes [59].
Table 3 compares the most problematic contaminants of both plastic wastes and tires. Heavy metal pollution requires the design of specific separation processes. Such designs allow for pyrolysis process development without increasing the risks of cancer and mental and renal conditions [60]. These factors are due to the environmental absorption of the emitted compounds. For example, if Ni passes through soil and then to food after pyrolysis, it increases the risk of lung cancer [61]. Ni accumulation leads to the necessity for the specific utilization of polymers that serve as stabilizing agents, such as acrylonitrile butadiene styrene (ABS), PP, LDPE and high-impact polystyrene (HIPS). Important solutions for the removal of metals and their reuse include adding a biomass such as wax [62].
Xu et al. [26,77] presented an efficient approach for Hg removal from coal that enables tire and plastic pyrolysis. Chlorine waste is a potential autocatalyst, as in the case of polypropylene or polyvinyl chloride (PVC) [78]. Organics usually can be reduced from metals by some fungi, but not in plastic form [79]. Tires are designed for extreme conditions and require more metals to obtain the desired properties. Thus, this results in waste becoming more polluted with metals. The metal contamination of polymers is a serious obstacle that needs to be overcome in design. Pyrolysis produces fewer toxins from cubic wastes than gasification but they are still present at hazardous concentrations [80]. More stabilizers are included in tires than in plastics, causing their pyrolysis to be less selective for benzene, toluene, xylene (BTX) conversion, and producing more ash [81]. Pollutant emissions in multistage pyrolysis were reduced by almost 90% by a nickel catalyst (5 wt% Ni/SiO2) [82].

3.2. Reactors Used in Pyrolysis of Plastic and Tires

The reactor’s selection for the pyrolysis process depends on economics and the final products to be synthesized from the wastes. More designs have been tested for the pyrolysis of waste tires than plastic, showing more relevant activity in waste tire utilization due to the requirement of larger spaces for storage [83]. A comparison of reactors is given in Table 4.
In Table 5, we provide an extension of Table 4 with the efficiency analysis. Fixed bed reactors are applied more often to reactions of one phase rather than other types of reactors. Plastic or tire pyrolysis selectivity depends on the form or size, as was shown for a different form of polypropylene [21].
These findings improved the design of efficient pyrolysis processes and methods for the quantification of polypropylene, polystirene and polyethylene in soil [97]. Tire waste pyrolysis usually generates more char than in the case of plastic wastes [81,90], while, in microwave-assisted reactors, it reaches 40.5% [21]. More types of reactors have been investigated for use in waste tire pyrolysis. Conical and fixed bed reactors are mostly used due to their feasible application [98,99]. These reactors are used commonly by different companies and are often applied if the desired products are gaseous products. In the case of the production of liquid or solid products, the most used are rotary kilns. Passaponti et al. [100] applied microwave pyrolysis for electrode production for alkaline fuel cells. The other types of reactors require more skill in controlling pollution. One of the most important demands of the reactors is an efficient product separation method, which can be obtained by applying the required swing pressure or membranes [101]. Therefore, microwave-assisted reactors are a promising method if various products of different, easily separable phases are the aim of the planned design. A comparison of the same reactor types used in pyrolysis is illustrated in Figure 1.
Reactor designs have different thresholds in bioprocesses and pyrolysis. In pyrolysis, projection requires a proper catalyst. In bioprocesses such as dark fermentation, the role of the catalyst is a bacterial enzyme. Therefore, reactions involve a bacterial body working in a chemical engineering ‘sense’ as microreactors [102,103]. Thus, pyrolysis is a simpler process, with more developed controlling tools [104,105,106]. Plastic and waste tire decomposition require much more energy, which is usually delivered with high heat (using a temperature increase) [40]. These temperatures disable enzymes and place force on catalysts, and stronger materials are required for reactor development [107]. A high temperature allows for the inexpensive application of swing pressure for the purification of gases, in contrast to bioprocesses [108,109].

3.3. Process Conditions

Asfand et al. [110] found that tires with cotton waste required less flash time than only tires, but this was longer than with cotton waste. In the case of polyethylene and polyolefin waste, the addition of cellulosic waste as paper improved the time and efficiency to 78% of liquid products, making it suitable for petrochemical usage, reducing halogen emissions by 50% in comparison to the case without paper addition [111]. According to [112], the energy produced during pyrolysis decreases as follows: MSW plastic > tires > HDPE > diesel. Therefore, the energy that is produced due to pyrolysis/combustion depends on the substrate or feed used in the process.
Catalytic and thermal pyrolysis can result in different properties of bio-oil [77] and a higher percentage of CO, CH4, C3H6, CO2 and C2H6 carbohydrates in the flue gas. The optimal temperature of HDPE pyrolysis is between 378 °C and 404 °C according to [113]. Waste tire pyrolysis can be also considered as the co-pyrolysis of mixtures of biopolymers and polymers, which is the initial problem in the pyrolysis of plastics without its separation by type. Such a mixture can provide a promising endothermic fuel, such as EHF-851 [114]. Some plastic composites are contaminated with metals, e.g., some electronic wastes, depending on the plastic type and varying in some pyrolysis requirements, such as activation energy [115]. According to [116,117], especially amorphous materials can bring more ash, being feasible for asphalt production. For Pe and PP, a mesoporous catalyst such as Al-Mn was found to be more efficient [118]. The composition of the products of waste tire pyrolysis depends on the temperature range, and the design of pyrolysis should consider applying, for example, a temperature of 400 °C for PET synthesis or a temperature range from 400°C to 650 °C for PET; see Figure 2.

3.4. Advantages and Disadvantages of Pyrolysis

Plastic pyrolysis is a method involving the fast utilization of waste that causes serious problems. Applying this method is the fastest way to avoid placing plastic/tires in solid municipal waste. The main issue is that there is a high energy demand. The design combinations of the pyrolysis process with solar energy are sufficient to maintain the energy demands, especially at the beginning of production. Otherwise, the process would be dependent on fossil fuels and would not be sustainable. The advantage of plastic and tire pyrolysis is the fast utilization of dangerous solid waste. Other benefits of pyrolysis are that it prevents the potential pathway of smart polymers, as conjugated polymers are difficult to produce from the bioprocesses; moreover, metals remaining from the process of production, such as catalysts or stabilizers, need to be removed as they inhibit the process, and the addition of a new catalyst is often needed. A low or even negative energy balance in the process, according to [19], becomes unprofitable.
Consideration of the problems of such processes is necessary when using an additional catalyst for pyrolysis. However, plastics and tires possess some catalyst and retardant residues, and they cannot be used for accelerating decomposition. The pyrolysis of tires causes high carbon monoxide emissions, preventing their replacement with natural gas as it is a source of methane [120,121]. However, this is suitable to be implemented for products obtained in Fisher–Tropsch processes. Matching polymer waste with a catalyst is a cost-generating problem that is easily solved [122]. Another problem with oil products involves the application contaminants, as they can be used only for industrial steam crackers and nanotubes [123]. Pyrolysis char is a promising filler for civil engineering or as an adsorbent for metal contaminants in wastewater [64]. Table 6 considers the selected examples of the dark fermentation of potato waste and wheat straw, and the pyrolysis of waste tires and PET (one of the most common plastic wastes). The yield of hydrogen production from the pyrolysis of both tires and PET is higher, being up to 8 and 11 times higher than the dark fermentation of wheat straw. In the case of plastic pyrolysis, the cost of production is slightly higher than that of potato waste. The pyrolysis of waste tires is more expensive than the use of PET or dark fermentation. Wheat straw dark fermentation requires expensive pretreatments, comparable to the catalyst costs and energy demand for plastic pyrolysis. Hydrogen production from PET pyrolysis is six-times less efficient than the use of polystyrene, according to [124]. Waste tire pyrolysis is high due to the necessity of the removal of metal frames, retardants and composite structures from many polymers and natural components, preventing tires from being damaged during exploitation. Pyrolysis is a much more efficient method for hydrogen production, needing much less waste and less area, thus lowering the price for 1 L of hydrogen production. Methane production is more efficient in dark fermentation or anaerobic digestion than in pyrolysis. The relevant problem is delivering renewable sources of heat, which can be obtained from photovoltaic or wind power [125], due to the high yield required to fulfil demands. Dark fermentation can utilize natural and food wastes and other biowastes (waste sewage, tannery waste, fats, lignocellulose, whey) that can provide an additional source of biohydrogen besides utilization.

3.5. Plastic Waste and Tire Life Cycle

According to [78], a green circular economy with the excellent usage of materials occurs when waste returns to the raw materials that have been produced. This design works in plastic and waste tires when it is transferred to other petrochemical materials (oil, chemical) and metal residues, which are separated or used as a catalyst again. The transformation of these wastes into oil leads to their direct use as energy carriers, which would be emitted then as simple gaseous products at non-toxic levels [87,133].
Pyrolysis of used tires and plastics can be adapted to produce biofuel, monomers, aromatics and nanomaterials. Naddeo et al. [134] designed special tires manufactured from easily recycled biopolymers to solve a contamination problem. The idea of circulating waste plastic or tires without considering metal separation is shown in Figure 3.
The decomposition of plastic and waste tires is simpler to control than bioprocesses. In dark fermentation, the control of the process and continuity is challenging due to difficulties in modeling [136], which are solved in the case of pyrolysis [137]. Pyrolysis’ kinetics is based on the Arrhenius equation, changing depending on the material and temperature, both in plastics [126] and tires [138]. In the case of bioprocesses’ equations, Gompertz and logistics are special modifications of the Arrhenius equation [139]. In the biological process, due to biological hydrogen production phenomena that single bacteria produce—usually as a metabolism byproduct generated periodically, while continuous production can be assumed only in a sufficiently numerous bacterial group—modeling algorithms are still in the test stage [140]. Thus, such phenomena can be interpreted as trigonometric dependences [141,142] or exponential [143,144]. For pyrolysis processes, authors have developed special programs and algorithms, such as the Aspen code, suitable for predicting, according to the heating values of plastics, the most efficient processes [122]. Waste tire pyrolysis simulations consider more factors by responding to heterogeneous components in the mixture, similar to the pyrolysis of a mixture of plastics [145].
The pyrolysis of plastic or tires is a method (see Figure 2) that seeks to obtain a petrochemical product as a chemical raw material, fuel or polymer chain monomers. After pyrolysis, these wastes can regain their usefulness. The process design requires the selection of a pyrolysis method focused on obtaining the selected products. For example, when there is a demand for the design of nanomaterial production, ultrasonic pyrolysis should be selected [146,147], while, in the case of BTX production, catalytical pyrolysis should be chosen [148].

4. Future of Pyrolysis Processes

Hydrogen is considered the fuel of the future, and the pyrolysis of plastic and tires is a method that is increasing this demand. The demand growth is bound with the implementation of more feasible storage solutions, as hydrides, including ammonia, allow the development of the conversion of wastes. According to Rasul et al. [149], the most promising advantages are ammonia’s easy storage and the feasible accumulation of hydrogen produced from pyrolysis and bioprocesses. Pyrolysis of plastic wastes and tires produces ash, which can be a source of materials for nanotechnology, with widespread application. The process allows the production of materials for photovoltaics and conjugated polymers (lowering their high price) that are more efficient in light absorption than silicon materials [150,151]. Pyrolysis requires little space and can be more mobile than bioprocesses. Therefore, feasible mobile reactors for pyrolysis could be applied to utilize local plastic wastes in dispersed environments—for example, pathways in national parks—to transform hazardous wastes [106,152]. This method could be applicable if membrane technology allows for the capture poisonous or hazardous gases and their separation into fine gases. Pyrolysis has developed faster in recent times due to the decrease in construction prices, decreasing by up to six times in 25 years [109,153]. According to Fivga [154], the promising biofuel potential of plastic and waste tire pyrolysis is important for the production of aviation fuels.
Smart proportions of pyrolysis reactors would make them suitable for use on ships or in other vehicles. These compatible designs would allow for the profitable elimination of plastic islands in oceans [155] and seas; immediate utilization is required to avoid the rapid contamination of seas with plastic and reduce the heavy metal pollution of the environment.

5. Conclusions

This review illustrated situations in which pyrolysis has more advantages than bioprocess, as well as reverse cases. In the case of artificial material wastes such as plastic or waste tires, biological processes are ineffective, while pyrolysis can be a helpful method of overcoming the problems of these wastes. Plastics and tires can be utilized in pyrolysis rapidly with the transfer of other desired products or energy carriers. The pyrolysis process reduces every type of organic waste, producing a broader variety of products than fermentation, but is more energy-demanding. Pyrolysis requires the separation of metals from plastics and tires to avoid the emission of toxic compounds and the use of expensive catalysts. The development of pyrolysis needs to overcome the production of products or energy by considering the equipment size, conditions, high energy demands and economic aspects. Pyrolysis of plastics permits a reduction in conventional material use for the production of polymers, especially smart or conductive, and organic nanomaterials are approached more commonly in building a new, sustainable living model suitable for the comfortable living of 7 billion people around the world, without environmental damage. Hydrogen production via the pyrolysis of plastics is up to 64% more efficient than from tires. Pyrolysis is more feasible in controlling and modeling than bioprocesses. Plastic waste pyrolysis can obtain up to 20 times more hydrogen from 1 kg of waste than dark fermentation. Waste tire pyrolysis methods can obtain up to 14 times more hydrogen than the biological approach. The pyrolysis of both wastes in an efficient and fast method for hydrogen production in comparison to other biological methods. The hydrogen production achieved by pyrolysis requires much less space than production using bioprocesses.

Author Contributions

G.S. performed all works of the research, supervised by F.A.Ö. and M.S. All authors have read and agreed to the published version of the manuscript.

Funding

The research was supported by the National Centre for Research and Development in Poland, under project no. BIOSTRATEG 3/344128/12/NCBR/2017, and the Institute of Fluid-Flow Machinery, Polish Academy of Science in Gdansk (grant number FBW-44—Solowski).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflict of interest.

Abbreviation List

PETpolyethylene terephthalate
HDPEhigh-density polyethylene
LLDPElinear low-density polyethylene
LDPElow-density polyethylene
PVCpolyvinyl chloride
PUpolyurethane
PApolyamides
PSpolystyrene
PPpolypropylene
ABSacrylonitrile butadiene styrene
HIPShigh-impact polystyrene
SNGsubstitute natural gas
BTXbenzene, toluene, xylene
HRThydraulic retention time
ZSM-5 catalystZeolite Socony Mobil-5
EHFendothermic hydrocarbon fuel
SBRstyrene–butadiene rubber

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Hydrogen 03 00034 g001 550
Figure 1. Comparison of fixed bed reactor for pyrolysis and dark fermentation.
Figure 1. Comparison of fixed bed reactor for pyrolysis and dark fermentation.
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Figure 2. Tire pyrolysis and conditions for the design of selected products [119].
Figure 2. Tire pyrolysis and conditions for the design of selected products [119].
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Figure 3. Life cycle from oil, composites and energy [135].
Figure 3. Life cycle from oil, composites and energy [135].
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Table
Table 1. Ash content of different plastics [19,20].
Table 1. Ash content of different plastics [19,20].
Ash contentPETHDPEPSPPLLDPE
No3%No2%No
Table
Table 3. Comparison of most common additives in tires and plastics.
Table 3. Comparison of most common additives in tires and plastics.
Metals and Pollutants [63]Tires [17]Plastics [64]RemarksReferences
AsPreservatives of natural rubberCatalysts in the HDPE processAs preservatives, they block decomposition. It is important to perform pyrolysis at the temperature of 650 °C to avoid the occurrence of gaseous oxides[65,66]
CdA thermal stabilizer of both natural and synthetic rubberCdS is a catalyst in the polymerization of PVC. Pigment in PE, PP, and PET. Occurs also in cable sheets and flooringThermal stabilizers that block pyrolysis. There is a need for an approach for the fast removal of Cd from tires and plastics for more economical and environmentally friendly pyrolysis.[67,68]
ChlorinePreservatives of natural rubberThe substituents of a polymer chainPyrolysis of PVC needs to overcome the coproduction of HCl in gaseous form.[69]
CrSupports polymerization of synthetic rubberMuch in HDPE, PVC, PP, PS, PET, PA, ABS, PU, LLDPEPolymerization residues block pyrolytic decomposition, a removal approach is needed[70,71]
Pb20 ppm on tire average, heat stabilizer of rubber in tire productionIn flooring, PVC, and dense plastics, LDPE is used as a heat stabilizer. average value of 247 ppmHeat stabilizer slows down pyrolysis; thus, efficient pyrolysis attempts need to remove it firstly[72,73]
HgCatalyst stabilizers in synthetic rubber for tiresHigh in vacuum cleaner bags, PVC, PP HDPE, PS.Heat stabilizers slow pyrolysis and poison catalyst[74]
NiCatalyst in tire productionStabilizer in production of HIPS, PP, LDPE, ABSStabilizer slows pyrolysis[75]
SbStabilizers of rubber and styrene in tire productionCatalysts in PET fibersCatalyst stabilizers[76]
Table
Table 4. Comparison of reactors for pyrolysis of waste tires and plastic.
Table 4. Comparison of reactors for pyrolysis of waste tires and plastic.
Type of WasteFixed Bed ReactorFluidized Bed ReactorConical Sparked BedMicrowaveAugerRotary KilnAblativeColumn
Waste TiresSuitable for fast pyrolysis, simple design and operation, high HRT, low heat transfer Optimal temperature for bus tires is 400 °CFast pyrolysis flash time from 1 s to 4 s, in slow 1–5 s. Enhances oil yield, high investment, design and operation costs.Fast heat transfer, suitable gas–solid contactEnhanced heat transfer operation under isothermal conditions. Good for production of absorbent carbon black Low HRT, good mass balance [84]Slow, simple design leads to small HRT, promising heat transfer [85]Fast for waste tires at experimental scale [18], suitable for catalytic pyrolysisGood for preparation of nanotubes; see Ahmad et al. [86]; suitable for ash preparation
PlasticsSuitable for nanoparticle production from HDPE and PVC [87]N2 flow reduction solved, vacuum product distributionWith more solid circulation, a coarse part can be processedPromising and effective heat transfer to plastic waste [88]Low HRT, good mass balanceNo useNo useGood for oxidant removal [89]
Table
Table 5. Comparison of the processes used due to different substrates.
Table 5. Comparison of the processes used due to different substrates.
Type of ProcessRaw MaterialEfficiencyRemarksReference
Catalytic process microwave-assistedHDPE chipsLiquid from 22% to 68%
Gas from 76% to 56%		Two-times higher ash yield than in the case of PP. Higher hydrogen, methane, ethylene, and ethane content of gas cases than in other cases. Much higher content (20%) of n-alkenes and n-alkanes.[21]
PP chipsGas 76%, liquid 24%Gas content has higher methane and hydrogen content than in pellet. Liquid content is mostly aromatics and cycloalkane, with 3% more polycyclic aromatic hydrocarbon and aromatics.
PP pelletLiquid products from 44.8% to 49%
Gas from 48% to 56%		Much more ash than in chips. High propylene level in liquid content.
LDPE chipsGas 47%, liquid 48%Addition of NiO catalysts, high in monocycled aromatics and hydrocarbon content in liquid phase, higher methane content from HDPE and PP[90]
Fortan® conical sparked bedWaste tires with removed metal cord-Liquid part with high content of monocycle aromatics and hydrocarbon up to 52%[91]
Fixed bed reactor heating rate 10 °C/minPSOil yield 88.5% (mostly aromatic compounds)Polymer catalyst (bentonite clay) ratio 0.05[92]
PPOil yield 90.5% (mostly nonaromatic compounds C13>)Polymer catalyst (bentonite clay) ratio 0.1
LDPEOil yield 87.6% (mostly nonaromatic compounds C13>)Polymer catalyst (bentonite clay) ratio 0.2
HDPEOil yield 88.9% (mostly nonaromatic compounds C13>)Polymer catalyst (bentonite clay) ratio 0.15
Horizontal tube
furnace		PVC37.3% ash yield90% removal of Cd and Zn was reached.[93]
Rotary kiln pyrolysisPE bottles39.7% of pyrolytic oilThe distilled product from pyrolytic oil from plastic waste has the potential to be used as a gasoline replacement fuel.[94]
Horizontal tube
furnace 750 °C		Waste tires with removed iron reinforcement42% char yield, 40% oil yield, 18% gas yieldThe parameters analyzed, which included the composition of the bio-oil, showed the presence of important chemicals that can be used as feedstocks and thermal conversion kinetics and to build a special waste recovery refinery[95]
Catalytic pyrolysis column reactor Pyro GerstelABSAromatic 85%, including 25% of BTEX, no ashZSM-5 catalyst (Zeolite Socony Mobil–5) containing 10% Ni[81]
PETAromatic 81%, including 12% of toluene, no ashNH4/ZSM-5
PPAromatic 78%, xylene 26.58%, total BTX 48.69% No ashNH4/ZSM-5
Tire waste SBR (styrene–butadiene rubber)Aromatic 37.82%, including 16.77% xylene, 14% ash, high efficiencyZSM-5 catalyst (Zeolite Socony Mobil–5) containing 10% Ni
Non-vulcanized SBRAromatic 68%, including 26.74% of BTX (10.49% xylene)NH4/ZSM-5
Tubular reactorPolyurethane43% liquidNa2CO3 as catalyst[96]
Two-stage reactor tubular and furnace reactorAutomotive seat foam consists mostly of polyurethane60% gaseous, 10% ashNickel catalyst (5 wt% Ni/SiO2)[82]
Table
Table 6. Comparison of hydrogen production from wheat straw and potato waste by dark fermentation and pyrolysis of waste tires and PET.
Table 6. Comparison of hydrogen production from wheat straw and potato waste by dark fermentation and pyrolysis of waste tires and PET.
Process TypeDark FermentationPyrolysis
SubstratePotato WasteWheat StrawWaste TiresPlastic PET [126]
Hydrogen yield in the experiment0.07 L of H2/g VSS [127]0.08 L of H2/g VSS [127]0.38 L of H2/g tire [128]0.29 L of H2/g PET [124]
The highest hydrogen yield published0.3 L of H2/g VSS [129].0.148 L of H2/g VSS [130]2.15 L of H2/g tire [131]3.32 L of H2/g PET [132]
Conditions in the selected studyMilled with a sieve 10 mmMilled with 10 mm sieve (knives were changed every 2 h of milling, pH 5.2)Minced to 5 mm, tube furnace quartz reactor Carbolite Gero® temperature 500 °C, sorbents: sodium hydroxide (15% solution), manganese oxide and zinc oxide [128]Catalyst Al2O3: supported by Ni catalyst Temperature 900 °C, two-stage processes using fixed bed reactor composed of stainless steel with diameter of 2.2 cm and height of 25 cm, process length 20 min [125]
Demand for process operation sufficient for the highest hydrogen productionMilling sieve 10 mm, stressing of inoculum, heating of reactor, pH 7.8Milling sieve 10 mm, stressing of inoculum, heating of reactor, pH 5.48Tire shredded to 6 mm, catalyst Al2O3:SiO2 supported by Ni catalyst, temperature 900 °C, a two-stage process using fixed bed reactor composed of stainless steel with diameter of 2.2 cm and height of 16 cm, process length 20 min [131]A commercial Ni/Al2O3 catalyst doped with Ca (Süd Chemie-G90LDP) conical spouted bed reactor at temperature 700 °C
Highest methane production yield in this study0.91 L/g VSS0.36 L/g VSS0.31 L/g waste tire [128]0.14 L/g PET [132]
Price of hydrogen production for optimal conditions; the current price was assumed as 0.18 $/kWh [75,76]1.61 $/mL H2 [75]16.62 $/mL H2 [76]29.21 $/mL H2 [131]1.79 $/mL H2 [124]
Price of hydrogen production in the study, the current price was assumed as 0.18 $/kWh0.62 $/mL H2 [73]5.8 $/mL H2 [73]9.97 $/mL H2 [128]3.21 $/mL H2 [132]
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Sołowski, G.; Shalaby, M.; Özdemir, F.A. Plastic and Waste Tire Pyrolysis Focused on Hydrogen Production—A Review. Hydrogen 2022, 3, 531-549. https://doi.org/10.3390/hydrogen3040034

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Sołowski G, Shalaby M, Özdemir FA. Plastic and Waste Tire Pyrolysis Focused on Hydrogen Production—A Review. Hydrogen. 2022; 3(4):531-549. https://doi.org/10.3390/hydrogen3040034

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Sołowski, Gaweł, Marwa Shalaby, and Fethi Ahmet Özdemir. 2022. "Plastic and Waste Tire Pyrolysis Focused on Hydrogen Production—A Review" Hydrogen 3, no. 4: 531-549. https://doi.org/10.3390/hydrogen3040034

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