Economic and Environmental Performance of an Integrated CO2 Refinery.

The consequences of global warming call for a shift to circular manufacturing practices. In this context, carbon capture and utilization (CCU) has become a promising alternative toward a low-emitting chemical sector. This study addresses for the first time the design of an integrated CO2 refinery and compares it against the business-as-usual (BAU) counterpart. The refinery, which utilizes atmospheric CO2, comprises three synthesis steps and coproduces liquefied petroleum gas, olefins, aromatics, and methanol using technologies that were so far studied decoupled from each other, hence omitting their potential synergies. Our integrated assessment also considers two residual gas utilization (RGU) designs to enhance the refinery's efficiency. Our analysis shows that a centralized cluster with an Allam cycle for RGU can drastically reduce the global warming impact relative to the BAU (by ≈135%) while simultaneously improving impacts on human health, ecosystems, and resources, thereby avoiding burden-shifting toward human health previously observed in some CCU routes. These benefits emerge from (i) recycling CO2 from the cycle, amounting to 11.2% of the total feedstock, thus requiring less capture capacity, and (ii) reducing the electricity use while increasing heating as a trade-off. The performance of the integrated refinery depends on the national grid, while its high cost relative to the BAU is due to the use of expensive electrolytic H2 and atmospheric CO2 feedstock. Overall, our work highlights the importance of integrating CCU technologies within chemical clusters to improve their economic and environmental performance further.

Trade-offs between Sustainable Development Goals in carbon capture and utilisation.

Carbon capture and utilisation (CCU) provides an appealing framework to turn carbon emissions into valuable fuels and chemicals. However, given the vast energy required to activate the CO2 molecule, CCU may have implications on sustainable development that are still poorly understood due to the narrow scope of current carbon footprint-oriented assessments lacking absolute sustainability thresholds. To bridge this gap, we developed a power-chemicals nexus model to look into the future and understand how we could produce 22 net-zero bulk chemicals of crucial importance in a sustainable manner by integrating fossil, CCU routes and power technologies, often assessed separately. We evaluated the environmental performance of these technologies in terms of their contribution to 5 Sustainable Development Goals (SDGs), using 16 life cycle assessment metrics and 9 planetary boundaries (PB) to quantify and interpret the impact values. We found that fossil chemicals could hamper the attainment of SDG 3 on good health and well-being and SDG 13 on climate change. CCU could help meet SDG 13 but would damage other SDGs due to burden-shifting to human health, water scarcity, and minerals and metals depletion impacts. The collateral damage could be mitigated by judiciously combining fossil and CCU routes with carbon-negative power sources guided by optimisation models incorporating SDGs-based performance criteria explicitly. Our work highlights the importance of embracing the SDGs in technology development to sensibly support the low-carbon energy and chemicals transition.

Process modelling and life cycle assessment coupled with experimental work to shape the future sustainable production of chemicals and fuels.

Meeting the sustainable development goals and carbon neutrality targets requires transitioning to cleaner products, which poses significant challenges to the future chemical industry. Identifying alternative pathways to cover the growing demand for chemicals and fuels in a more sustainable manner calls for close collaborative programs between experimental and computational groups as well as new tools to support these joint endeavours. In this broad context, we here review the role of process systems engineering tools in assessing and optimising alternative chemical production patterns based on renewable resources, including renewable carbon and energy. The focus is on the use of process modelling and optimisation combined with life cycle assessment methodologies and network analysis to underpin experiments and generate insight into how the chemical industry could optimally deliver chemicals and fuels with a lower environmental footprint. We identify the main gaps in the literature and provide directions for future work, highlighting the role of PSE concepts and tools in guiding the future transition and complementing experimental studies more effectively.

Hybridization of Fossil- and CO2 -Based Routes for Ethylene Production using Renewable Energy.

Carbon capture and utilization (CCU) has recently gained broad interest in the chemical industry. Direct electro- and thermocatalytic technologies are currently the focus of intense research, where the former employs electricity directly to reduce the CO2 molecule, while the latter comprises hydrogenation of CO2 in tandem with electrocatalytic water splitting. So far, it remains unclear which of the two is superior, yet this information is considered critical. Focusing on the platform chemical ethylene, the two CCU routes were compared using state-of-the-art performances with the fossil technology considering different power and CO2 sources. The thermo-route was found to be, at present, economically and environmentally better, yet under the same electrolyzer efficiencies, the electro-route would become superior. CCU routes could substantially improve the carbon footprint of the fossil ethylene (by 236 %) while decreasing at the same time impacts on human health, ecosystem quality, and resources (64, 140, and 80 %, respectively). However, they are economically unattractive even when considering externalities (indirect cost of environmental impacts), that is, 1.7- to 3.9-fold more expensive compared to the current fossil-based analogue. Acknowledging this limitation, the concept of hybridization was applied as a means to smooth the transition towards more sustainable chemicals. Accordingly, it was found that an optimal hybrid plant could produce carbon-neutral (cradle-to-gate) ethylene with a premium of only 30 % over the current market prices by judiciously combining CCU routes with fossil technologies.