Abstract
Rapid industrialization and urbanization have increased the demand for both energy and mobility services across the globe, with accompanying increases in greenhouse gas emissions. This short paper analyzes strategic measures for the abatement of CO2 emissions from oil refinery operations. A case study involving a large conversion refinery shows that the use of post-combustion carbon capture and storage (CCS) may only be practical for large combined emission point sources, leaving about 30% of site-wide emissions unaddressed. A combination of post-combustion CCS with a CO2 capture rate well above 90% and other mitigation measures such as fuel substitution and emission offsets is needed to transition towards carbon-neutral refinery operations. All of these technologies must be configured to minimize environmental burden shifting and scope 2 emissions, whilst doing so cost-effectively to improve energy access and affordability. In the long run, scope 3 emissions from the combustion of refinery products and flaring must also be addressed. The use of synthetic fuels and alternative feedstocks such as liquefied plastic waste, instead of crude oil, could present a growth opportunity in a circular carbon economy.
1 Introduction
The Sixth Assessment report from the Intergovernmental Panel on Climate Change (IPCC) finds that limiting global average temperature rise to 1.5ā2°C from 1850 is unlikely without material reductions in greenhouse gas (GHG) emissions (). This sets an imperative to drastically reduce emissions from economic activities globally, whilst improving access to energy and ensuring its affordability.
Owing to its role as a provider of transport fuels and chemicals, the global refining sector has increased its capacity by 13% over the period from 2000 to 2018, with a corresponding increase in total GHG emissions by 24% (). In total, oil refineries contributed 4% to global CO2 emissions in the year 2018, equating to approximately 1.3Ā Gt CO2. Although the demand for refined petroleum products has been declining in Europe and Latin America, a significant growth is seen in India and China, in part driven by rapid industrialization and an increasing demand for mobility services (; ). By 2025, over 150 additional refineries are planned to be operational across Asia, the Middle East, and Africa (), thereby posing an inherent challenge to carbon-neutrality ().
A cost-effective emission mitigation strategy needs to be developed for refineries to be operable in a net-zero society. The nub of the argument in this paper is that a combination of post-combustion CO2 capture and storage (CCS) with fuel switching could provide the basis for such a strategy, considering both economic and environmental trade-offs. This ensures that scarcer greenhouse gas removal services (e.g., afforestation, direct air capture of CO2) are utilized to offset the most challenging sources of emissions in the economy, and not as the principal means to mitigation (). A key consideration is that CO2 capture rates well above 90% are necessary to achieve a sufficiently high CO2 avoidance using post-combustion CCS because of upstream impacts from the fuel supply chains. Furthermore, it is important to minimize environmental burden shifting for any net-zero strategy to achieve sustainable deployment.
2 Emission Sources in a Large Conversion Refinery
There are more than a thousand oil refineries worldwide today, categorized broadly as hydroskimming or larger conversion refineries. Hydroskimming refineries comprise distillation units, and a series of process units to produce petrol, jet fuel, and middle distillates. By contrast, larger conversion refineries include hydrocrackers and catalytic cracking units to further reduce heavier crude fractions into lighter products (). These constitute over 70% of all refineries in Europe and the United States, and emit around four times as much CO2 per barrel of oil as the simpler conversion refineries ().
The main emission sources in larger conversion refineries are, in order of importance, the power station (29% of total emissions in an average refinery), fluid catalytic cracking unit (19%), atmospheric distillation units (19%), and steam methane reformer for hydrogen production (11%) (). The refinery flow diagram in Figure 1A shows the key conversion processes and outputs. Nowadays, the power station often consists of a natural gas combined cycle (NGCC) plant with additional gas-fired boilers to cover the overall power requirements of the refinery. Similarly, the heat requirements of the atmospheric and vacuum distillation units are met by burning the fuel oil and gases. The steam methane reformer uses natural gas both as a feedstock and a fuel, producing two separate CO2 point sources that add up to about 10 kgCO2,eq for each kg of hydrogen produced.
FIGURE 1
Smaller units such as heaters, boilers, and gas turbines are also commonly powered by fuel gases, fuel oil, or natural gas. These heterogeneous emission point sources have a relatively low CO2 concentration (around 8%vol), but may emit large quantities of CO2 altogether. They are often distributed across a refineryās site, as illustrated in Figure 1B, forming clusters that are separated over distances of several hundred meters or more (
A breakdown of emission point sources in a typical larger conversion refinery (Figure 1B) is provided in Supplementary Table S1 of the Electronic Supplementary Material (ESI), including an estimated CO2 concentration for each stream. Given these characteristics, the next section reviews the principal CO2 abatement measures, either approaches or technologies for reducing the CO2 footprint of assets, followed by an assessment of their suitability for deployment in this sector to meet net-zero targets in the final section.
3 Carbon Mitigation in Refineries
This section summarizes the main strategic measures to drive down direct CO2 emissions in oil refineries.
3.1 Energy Efficiency
Energy efficiency improvements are regarded by many as a cost-effective mitigation strategy (
3.2 Carbon Capture and Storage
The oil and gas sector was an early adopter of CCS technology since the 1970s for enhanced oil recovery (EOR), which has provided a foundation of experience for deployment in other CO2 mitigation applications. A large body of research thereof has examined the use of CCS technology for mitigating emissions in refineries (
3.3 Fuel Switching
Since around 70% of a refineryās emissions are the result of fuel combustion (
4 Discussion
4.1 Why Use a Multipronged Approach?
The net-zero paradigm entails balancing any residual CO2 emissions with an equivalent amount of permanent CO2 removal from the atmosphere. Because of large uncertainties in the cost of technologies such as direct air capture (DAC) (
The CO2 avoidance is defined as the quantity of CO2 emissions avoided using abatement measures relative to a reference plant which uses a given mix of fuels and technologies. It is clear that both scope 1 (direct emissions from owned or controlled assets) and scope 2 emissions (indirect emissions from utilities, electricity, heating and cooling) need to be an integral part of any CO2 avoidance assessment in order for strategic decisions to be fully aligned with net-zero ambitions. An increase in the CO2 capture rate of the CCS plant generally goes in hand with an increase in overall (absolute) energy consumption and thus indirect environmental impacts (
Here, we discuss the merits and caveats of post-combustion CCS in a highly optimistic case where all point-source emissions of the model refinery from Figure 1B would be captured. The case study assumes that the CCS unit would be powered by a dedicated CHP plant, any CO2 emissions of which would also be directed to the CCS unitāa realistic scenario insofar as installing CCS in existing refineries would entail retrofits, yet excess utilities (steam and electricity) might not be available on-site in most refineries. Further details about the case study assumptions and calculation procedure are reported in Section 3 of the ESI for completeness.
The first scenario in Figure 2A considers a natural gas-fired CHP plant. Notice how achieving 90% CO2 avoidance requires a capture rate in the CCS unit greater than 96% when natural gas from Great Britain fuels the CHPāa discrepancy attributed to upstream emissions from the natural gas supply chain as aforementioned. Conversely, a 99% capture rate in the CCS unit delivers 86% and 79% CO2 avoidance when the CHP fuel corresponds to natural gas and LNG, respectively, both at the global average emissions intensity. To put it in perspective, for our model refinery where post-combustion CCS covers 72% of the direct CO2 emissions (Figure 1B and Supplementary Table S1), the CO2 avoidance with a CHP plant fired by natural-gas at the global average emissions intensity and a 99% CO2 capture rate is no more than 62%. This reinforces the need for complementary measures such as fuel switching and negative emissions technologies, in addition to reducing scope 2 emissions. Another important consideration is that the post-combustion CCS unit consumes around 0.13 tonnes of natural gas per tonne of CO2 at capture rates of 90% and above, thus significantly increasing the primary energy requirements of a refinery.
FIGURE 2

Interplay between CO2 avoidance rate (color map and contour lines), CO2 capture rate (x-axis), and scope 2 emissions intensity (y-axis) in post-combustion CCS. (A): Scenario of a CCS unit powered by a natural gas-fired CHP plant, with all its exhaust gases directed to the CCS unit. The dashed horizontal line labelled GB indicates natural gas from Great Britain; those labelled Global average and LNG depict natural gas and liquefied natural gas mix, respectively, at the global average emissions intensity. (B): Alternative scenario of a CCS unit powered by a hydrogen-fired CHP plant. The two dashed lines labelled Blue correspond to hydrogen produced via steam reforming of natural gas from Great Britain or LNG at the global average emissions intensity, both assuming a 90% CO2 capture rate from the reformer flue gas; the line labelled Green considers water electrolysis powered by wind electricity. Refer to Section 3 of the ESI for details about the underlying assumptions and the calculation procedure.
For comparison, the second scenario in Figure 2B considers a hydrogen-fired CHP plant. Observe how scope 2 emissions (y-axis) attributed to blue (methane-derived with CCS) hydrogen increase compared to those of natural gas. Under the assumption of a 90% CO2 capture rate in the blue hydrogen production process, they are predicted to triple in the case of natural gas from Great Britain and almost double in the case of LNG at the global average emissions intensity. This supports the conclusion that burning natural gas in the CHP plant and capturing the resulting CO2 emissions would be more effective than switching to hydrogen fuel, unless this substitution fuel has a low indirect emission intensity as for instance with green (electrolytically-derived using renewable power) hydrogen. If blue hydrogen (generated from a global average supply of natural gas with a 90% CO2 capture rate) was used to address the remaining 28% of the direct emissions from the model refinery, the overall CO2 avoidance would increase from 62% to 75%; this would further increase to 87% if green hydrogen was used instead. To achieve net-zero, around 13ā25% of the refineryās direct emissions would still need to be offset through CO2 removal technologies.
The broader implications of producing green hydrogen to fuel the CHP plant of a refinery should also be considered carefully. In particular, guaranteeing a continuous supply of green hydrogen would require hydrogen storage, increasing cost. Moreover, green hydrogen suffers higher conversion losses compared to renewable electricity, and switching to renewable electricity could thus allow for greater CO2 avoidance rates. This cursory analysis points to the need for a detailed techno-economic analysis and life-cycle assessment between renewable electricity, green hydrogen, and blue hydrogen as future energy vectors in refineries.
4.2 Future Prospects
The previous discussion has underlined the need for a combination of emission mitigation strategies to effectively decarbonize existing oil refineries, taking the best of post-combustion CCS and fuel switching and complementing with CO2 removal technologies. Newer refinery installations could benefit further from the use of low-carbon power sources, such as solar or wind electricity, as the power plant typically is the single largest point-source emitter. Concentrated solar power (CSP) systems can already operate at steam temperatures between 60 and 250°C and have the ability to reach temperatures beyond 400°C (
Incorporating CCS in any application causes some degree of environmental burden shifting. The additional energy and infrastructure requirements, along with the consumption of additional resources (e.g., MEA solvent), increase water consumption and smog formation among other environmental impacts (
A major focus herein has been on addressing scope 1 and 2 emissions from refineries, in the manner of a well-to-tank analysis. Yet these activities may only account for 10ā20% of emissions from oil products, while the remaining 80ā90% is associated with fuel use (
Besides DAC, engineered CO2 removal technologies include the use of biogenic carbon feedstock with CCS for bioenergy production, also known as BECCS (
More generally, CO2 utilization may be financially viable in a supportive market environment but commercially available utilization technologies are still lacking the scale and permanence of CO2 removal required to be relevant for long-term climate stabilization (
Finally, the sustainability of CO2 mitigation strategies in refineries ought to consider the social dimension alongside economic and environmental trade-offs. This could follow a triple helix approach, as recently advocated for CO2 utilization assessment (
Statements
Data availability statement
The original contributions presented in the study are included in the article/Supplementary Material, further inquiries can be directed to the corresponding authors.
Author contributions
ConceptualizationāAB, NS. Writing (original draft)āAB, MB, DD, AG-G, NS. Writing (review and editing)āAB, MB, BC, DD, AG-G, NS. VisualizationāMB, DD, NS. SupervisionāBC.
Acknowledgments
AB and BC are grateful to the Engineering and Physical Sciences Research Council (EPSRC) for funding the research under the UKRI Interdisciplinary Centre for Circular Chemical Economy programme (EP/V011863/1). DD would like to acknowledge EPSRC funding under the United Kingdom Carbon Capture and Storage Research Centre (UKCCSRC, EP/P026214/1). MB would like to acknowledge RCUK funding under grants EP/T033940/1 (CCS Project), NE/P019900/1 (GGR Opt), EP/M001369/1 (MESMERISE-CCS), EP/N024567/1 (CCSInSupply) and EP/M015351/1 (ONF).
Conflict of interest
The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.
The handling Editor declared a past co-authorship with the authors MB, NS.
Publisherās note
All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article, or claim that may be made by its manufacturer, is not guaranteed or endorsed by the publisher.
Supplementary material
The Supplementary Material for this article can be found online at: https://www.frontiersin.org/articles/10.3389/fceng.2022.804163/full#supplementary-material
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Summary
Keywords
refinery, decarbonization, CCS, fuel switching, hydrogen, oil, net-zero
Citation
Sunny N, Bernardi A, Danaci D, Bui M, Gonzalez-Garay A and Chachuat B (2022) A Pathway Towards Net-Zero Emissions in Oil Refineries. Front. Chem. Eng. 4:804163. doi: 10.3389/fceng.2022.804163
Received
28 October 2021
Accepted
13 January 2022
Published
11 February 2022
Volume
4 - 2022
Edited by
Matteo Gazzani, Utrecht University, Netherlands
Reviewed by
Qingchun Yang, Hefei University of Technology, China
Mar PƩrez-Fortes, Delft University of Technology, Netherlands
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Copyright
Ā© 2022 Sunny, Bernardi, Danaci, Bui, Gonzalez-Garay and Chachuat.
This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.
*Correspondence: Andrea Bernardi, a.bernardi13@imperial.ac.uk; BenoƮt Chachuat, b.chachuat@imperial.ac.uk
This article was submitted to Computational Methods in Chemical Engineering, a section of the journal Frontiers in Chemical Engineering
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All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations, or those of the publisher, the editors and the reviewers. Any product that may be evaluated in this article or claim that may be made by its manufacturer is not guaranteed or endorsed by the publisher.