Integrated Catalytic Recycling of Plastic Residues Into Added-Value Chemicals

Project Information

iCAREPLAST

Grant agreement ID: 820770

DOI

10.3030/820770

Project closed

EC signature date 3 August 2018

Start date 15 October 2018

End date 14 April 2023

Funded under

• INDUSTRIAL LEADERSHIP - Leadership in enabling and industrial technologies - Advanced manufacturing and processing

Total cost

€ 8 085 682,50

EU contribution

€ 6 507 043,25

Coordinated by

AGENCIA ESTATAL CONSEJO SUPERIOR DE INVESTIGACIONES CIENTIFICAS
Spain

Periodic Reporting for period 3 - iCAREPLAST (Integrated Catalytic Recycling of Plastic Residues Into Added-Value Chemicals)

Reporting period: 2021-10-15 to 2023-04-14

Summary of the context and overall objectives of the project

iCAREPLAST provides a cost and energy-efficient alternative to recycle and valorise non-recycled plastic waste (~70% Europe) that is currently sent to landfills (27%) or incinerated (42%). The process combines pyrolysis, catalytic treatment and membrane technologies to obtain high added-value chemicals, such as aromatics (BTXs and alkylaromatics), that can produce virgin-quality polymers. To ensure efficiency and sustainability of the process, advanced control techniques are applied to harmonise economic and environmental targets, using indicators defined, taking into account LCA and LCC analyses. Hydrocarbon-rich side-streams are recovered for energy valorisation via oxycombustion integrated with CO2 capture, improving energy sustainability and avoiding GHG emissions. The valorisation of by-products (char, CO2) contributes to economic sustainability of the process and avoids waste generation.
iCAREPLAST achieved enhanced plastic upcycling efficiency at pilot-plant scale (TRL-7). The process has resulted in a quantifiable 12% increment in pyrolysis liquid yield, 45% reduction in energy requirements, and 95% reduction in residues. These improvements have a great impact on the economic yield of the process, resulting in an increase of up to 200%.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

All project objectives were achieved. The waste plastic raw materials were fully characterised macro and microscopically, and the pre-treatment operations were designed. The waste plastic mixture was optimised and selected to achieve high liquid yields with an adapted molecular composition. Thermal and catalytic pyrolysis tests were carried out in different reactors resulting in high liquid yields and thus maximising the content of the products. The suitability of the membranes was tested using a model mixture representing the mixture that could be obtained after pyrolysis or alkylation. Alkylation, aromatisation, and oxycombustion tests were out at lab-scale. The integration of the pre-treatment line and the solid extraction unit with the pyrolyser, the modifications of the catalytic reactor to the aromatization process and the installation of a bench-scale distillation unit were carried out. Pyrolysis tests were performed under different conditions to investigate their effect on the reaction rate, product distribution, and product quality. A pilot-scale aromatization test was conducted using the light fraction distilled from the pyrolysis liquids produced under optimal conditions and an industrial zeolitic catalyst based on ZSM-5. The steady state model of the entire iCAREPLAST process was completed. The LCA models were completed to assess environmental sustainability and LCC to include cost parameters. Market and techno-economic analyses of linear alkylbenzenes production and commercialization of BTXs, CO2 and char were carried out.
Communication and dissemination efforts included presentations at events, conferences, and fairs, as well as scientific publications. Training activities engaged students at various academic levels. iCAREPLAST is positioned within the future plastic circularity landscape, with the Project Coordinator playing a leading role in the Plastics Circularity Multiplier group.
Developed an exploitation plan to assess iCAREPLAST technologies' economic potential and market uptake. Key factors include a production capacity of 12,000,000 kg/year, a €25,000,000 investment, inflation rates, a 15-year analysis period, material and energy balance based on experiments and modelling optimization, and by-product sales (e.g. €1/kg from aromatics). The results indicate potential revenue streams and project profitability, considering these factors and market prices for generated by-products.
iCAREPLAST significantly contributes to CO2 emission reduction. The treatment of mixed plastic waste resulted in a positive impact of -0.3 kg CO2-Eq. This is achieved by substituting secondary products for those produced from virgin fossil fuels. The project included a TRL5 unit that allowed for the capture and energy valorisation of fuel-gas streams at various process points through oxycombustion, which increased the overall energy efficiency. Analyses developed revealed that energy efficiency could be improved by more than 93% compared to current recycling processes.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

The project demonstrates the whole technology for plastic waste valorisation in a pilot plant able to process >100 kg/h of plastic. It offers an efficient and sustainable chemical process utilising non-recycled plastic waste as starting material. Compared with existing chemical recycling technologies for plastic wastes, iCAREPLAST contributes to: (i) improve pyrolysis liquid yield up to 12% (increment), which with the selected plastics mixture, at the pilot scale, the liquid yields obtained ranged from 76-84%; (ii) reduce energy requirements up to 45%. It has been shown that when energy criteria are considered, the pyrolysis process can be run saving approximately 0.36 MJ/kg of treated plastic and obtaining similar liquid pyrolysis yields. Similar conclusions have been obtained for the joint operation of pyrolysis plus alkylation. Preliminary models, including oxycombustion, give an optimistic view in which the energy balance of the entire process is negative (energy is recovered); (iii) reduce residue production up to 95%. Residue production from pyrolysis step is estimated less than 0.05 %. Moreover, the membrane separation tests are key aiming to maximize the products yield and to minimize the residue production of the integrated solution; and (iv) increase economic yield up to 200%.
iCAREPLAST process reduce CO2 emissions for plastic waste treatment compared to conventional incineration. When considering the substitution of virgin by secondary materials, the impact of the recycling process can even reach below net zero level. The oxycombustion unit (TRL5) for the capture and energy valorisation of fuel-gas streams significantly increased the overall energy efficiency. The environmental assessment of the recycling process can be carried on continuously in the future through the developed Live LCA framework and can be used as a decision support tool for further process optimization.
iCAREPLAST expand the spectrum of plastic waste types that can be recycled to almost every plastic. Thus, when no restrictions are put on the plastic materials that can be recycled, citizens will receive a message that will reinforce their involvement in the recycling chain. This citizen engagement will contribute to the EU targets for recycling 65% of municipal waste and 75% of packaging waste by 2030.
iCAREPLAST achieved important results by developing and implementing new methods: a new pre-treatment process for plastic blends, an advanced char extraction system, tools for analysing ecological performance in real-time, an innovative unit for separating aromatic products, an oxycombustion unit for side stream gases, a new alkylation catalyst, catalytic processes in plastic-mixture pyrolysis, a control architecture for optimizing pyrolysis yield, and a real-time monitoring LCA application.
The pilot-plant scale process has demonstrated (TRL-7) been successful in increasing the efficiency of plastic upcycling (a 12% increase in pyrolysis liquid yield, a 45% reduction in energy requirements, and a 95% reduction in residues), which resulted in a significant improvement of the economic yield of the process (up to 200% increase compared to current processes).

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