Publications
185 results found
Wong JJ, Iruretagoyena D, Shah N, et al., 2023, A three-interface random pore model: The reduction of iron oxide in chemical looping and green steel technologies, Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol: 479, ISSN: 1364-5021
Accurate modelling of the gaseous reduction of porous iron oxide powders or fines is important in industry for (i) reinventing the carbon intensive production of iron and steel and (ii) chemical looping technologies in the sphere of carbon capture and storage. A new three-interface random pore model is derived and applied to the gaseous reduction of hematite (Fe2O3) to iron (Fe). The structural reaction-diffusion model is able to describe three simultaneously reacting oxide layers, Fe2O3, magnetite (Fe3O4) and wustite (FewO). The geometric nature of the model encodes structural information about the particles (porosity, surface area, pore length and size distribution), measured here by experiment. The model is usefully able to separate structural particle properties from individual rates of reaction and product layer diffusion. The results have been compared and fitted to thermogravimetric experiments between 800-1000∘ C and three CO/CO2 gas mixtures. Rate constants for each indvidual reaction have been obtained and fit well to Arrhenius plots. The reduction of Fe2O3-Fe3O4 was controlled by diffusion and reaction kinetics, while the reduction of Fe3O4-FewO and FewO-Fe was limited by reaction kinetics. Metallization rates of the iron oxide powders were rapid, showing promise for both hydrogen-based direct reduced iron and chemical looping processes.
Eluwah C, Fennell PS, Tighe CJ, et al., 2023, A novel technological blue hydrogen production process: industrial sorption enhanced autothermal membrane (ISEAM), Energy Advances, Vol: 2, Pages: 1476-1494, ISSN: 2753-1457
A novel technological industrial blue hydrogen production process – the Industrial Sorption Enhanced Autothermal Membrane (ISEAM) process, with the potential to produce constant fuel cell grade hydrogen with a purity of 99.99%, regardless of upstream process upsets, has been modelled using an Aspen Plus simulator and MATLAB (including both thermodynamics and kinetics analysis). The process exhibits a very high hydrogen yield (99%), and methane conversion (99.9%), with a low carbon monoxide footprint (at ppm levels). The results were validated by comparing against experimental data published in the literature. Parametric evaluations were later conducted to identify the optimal operating conditions for the developed blue hydrogen ISEAM process. The required reforming heat is provided by the exothermic carbonation reaction of a sorbent, while chemical looping of the oxygen carrier (metal oxides) provides the regeneration heat required for the saturated sorbent, in a novel multi-tubular packed shell and tube reactor. Pinch analysis shows that the process is auto thermal (so it does not need any external heating utility) and can achieve an extremely high 97.5% thermal and hydrogen production efficiency. The ISEAM process was benchmarked against an industrial steam methane reforming (SMR) plant and the result shows ≥32% improvements in most of the technical parameters that were evaluated. Economic evaluation shows a levelized cost of hydrogen (LCOH) of $2.6 per kg-H2 for the baseline SMR plant compared with $1.3 per kg-H2 for the ISEAM process (a 50% cost reduction). The cost of CO2 removal (CCR) was calculated as $180 per tonneCO2 for the baseline SMR process compared with $33.2 per tonneCO2 (81.6% cost reduction) for the novel process. The novel ISEAM process utilizes mature and existing industry technologies such as desulphurization, pre-reforming, adsorption, membranes, waste heat boilers, and pressure swing adsorption. Because of this, scale-up is easier and
High M, Song Q, Campbell KLS, et al., 2023, Layered double hydroxide‐derived copper‐based oxygen carriers for chemical looping applications: oxygen release kinetics and impact of loading on long‐term performance, Greenhouse Gases: science and technology, Vol: 13, Pages: 505-545, ISSN: 2152-3878
Chemical looping with oxygen uncoupling, a variant of chemical looping combustion, requires chemically and physically stable oxygen carriers over long-term redox cycling. Copper-based oxygen carriers are characterised by high oxygen release rates but experience sintering at high temperatures. The use of layered double hydroxides (LDHs), prepared via co-precipitation, as oxygen carrier precursors has been shown to effectively limit deactivation of copper-based mixed metal oxides (MMOs) over extended redox cycling. The LDH-derived MMOs have highly dispersed metal oxide within a stable support; the high dispersion of metals is due to the LDH precursor structure. In this work, a fluidised bed reactor (FBR) was used to study the intrinsic kinetics of oxygen release from CuO/MgAl2O4 oxygen carriers synthesised via the LDH-MMO design strategy. The long-term performance of MMOs with higher loadings of CuO, calcined from LDHs with higher Cu contents, was also investigated using an FBR. The intrinsic kinetics were determined using a kinetic model incorporating an effectiveness factor. By minimising the effects of intra- and inter-particle mass transfer, the activation energy and the pre-exponential factor of the lower loading MMOs were determined to be 51 ± 3 kJ mol−1 and 0.0567 s−1, respectively. All MMOs showed excellent stability over 100 redox cycles in a thermogravimetric analyser. However, the pH during co-precipitation of the LDHs affected the stability of the MMOs in an FBR. The MMOs calcined from LDHs synthesised at pH 9.5 disintegrated during operation, whilst those produced from LDHs synthesised at pH 11 maintained high conversion and physical integrity over 100 redox cycles. © 2023 The Authors. Greenhouse Gases: Science and Technology published by Society of Chemical Industry and John Wiley & Sons Ltd.
Corona JJM, Campbell KS, Fennell PSS, 2023, Enhancement of iron-based oxygen carriers through alloying with tungsten oxide for chemical looping applications including water splitting, GREENHOUSE GASES-SCIENCE AND TECHNOLOGY, Vol: 13, Pages: 565-574, ISSN: 2152-3878
Zhang Z, Wong JJ, Scott SA, et al., 2023, Spouted fluidised bed reactor for kinetic measurements of the reduction of Fe2O3 in a CO/CO2 atmosphere part II: An extended random pore model for solid-state diffusion, CHEMICAL ENGINEERING RESEARCH & DESIGN, Vol: 194, Pages: 597-609, ISSN: 0263-8762
Iruretagoyena D, Fennell P, Pini R, 2023, Adsorption of CO2 and N2 on bimetallic Mg-Al hydrotalcites and Z-13X zeolites under high pressure and moderate temperatures, CHEMICAL ENGINEERING JOURNAL ADVANCES, Vol: 13, ISSN: 2666-8211
Leonzio G, Mwabonje O, Fennell PS, et al., 2023, Corrigendum to “Environmental performance of different sorbents used for direct air capture” [Sustain. Prod. Consum. 32 (2022) 101–111], Sustainable Production and Consumption, Vol: 36, Pages: 415-415, ISSN: 2352-5509
Weihs GAF, Jones JS, Ho M, et al., 2022, Life cycle assessment of co-firing coal and wood waste for bio-energy with carbon capture and storage - New South Wales study, ENERGY CONVERSION AND MANAGEMENT, Vol: 273, ISSN: 0196-8904
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- Citations: 5
Driver JG, Hills T, Hodgson P, et al., 2022, Simulation of direct separation technology for carbon capture and storage in the cement industry, CHEMICAL ENGINEERING JOURNAL, Vol: 449, ISSN: 1385-8947
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- Citations: 1
Leonzio G, Fennell PS, Shah N, 2022, Air-source heat pumps for water heating at a high temperature: State of the art, Sustainable Energy Technologies and Assessments, Vol: 54, Pages: 1-22, ISSN: 2213-1388
Concerns about climate changes are urging the decarbonisation of the energy sector and heat pumps are evaluated for this purpose here. About half of total energy consumption is caused by heating, and the use of heat pumps for this aim is gaining the attention of the research community.This work shows a comprehensive overview of air-source heat pumps used for water heating at a high temperature, with a particular aim to add the supplied heat into the air capture cycle. Air-source heat pumps use different cycles. The literature analysis shows that high temperatures (up to 90 °C) can be easily achieved by trans-critical cycles, while innovative schemes based on heat recuperative solutions might provide hot water up to 99 °C. Very few studies have been conducted about absorption cycles, although these can potentially ensure higher temperatures for the supplied water (up to 115 °C).Although real industrial air source heat pumps achieve a water temperatures lower than those reported above, their utilization is encouraged because, even at high temperatures (up to 100 °C), there are primary energy consumption, cost and carbon dioxide emission savings compared to a traditional boiler, especially when the renewable electricity is used.
Sendi M, Bui M, Mac Dowell N, et al., 2022, Geospatial analysis of regional climate impacts to accelerate cost-efficient direct air capture deployment, One Earth, Vol: 5, Pages: 1153-1164, ISSN: 2590-3322
Carbon dioxide (CO2) removal from the atmospheric will be essential if we are to achieve net-zero emissions targets. Direct air capture (DAC) is a CO2 removal method with the potential for large-scale deployment. However, DAC operational costs, and thus deployment potential, is dependent on performance, which can vary under different climate conditions. Here, to further develop our understanding of the impact of regional climate variation on DAC performance, we use high-resolution hourly based global weather profiles between 2016 and 2020 and weighted average capital costs to obtain DAC regional performance and levelized cost of DAC (LCOD). We found that relatively cold and drier regions have favorable DAC performance. Moreover, approximately 25% of the world’s land is potentially unsuitable due to very cold ambient temperatures for a substantial part of the year. For the remaining regions, the estimated LCOD is $320–$540 per tCO2 at an electricity cost of $50 MWh−1. Our results improve the understanding of regional DAC performance, which can provide valuable insights for sustainable DAC deployment and effective climate action.
Leonzio G, Fennell PS, Shah N, 2022, Modelling and analysis of direct air capture systems in different locations, Chemical Engineering Transactions, Vol: 96, Pages: 1-6, ISSN: 1974-9791
Direct air capture is an important negative emission technology with the aim to reduce carbon dioxide emissions in the atmosphere and to face the current environmental problems such as global warming and climate change. This emerging technology can be based on an adsorption system affected by the used sorbent (physisorbents or chemisorbents). Efficiencies can be measured through the use of key performance indicators that allow a comparison among different processes. An independent analysis was conducted in our previous research to evaluate key performance indicators (total cost, energy consumption, environmental impact and capture capacity) for a direct air capture system based on adsorption using different sorbents (three metal organic frameworks and two amine functionalized sorbents). In this research, the same analysis was extended to several Countries around the world, changing the ambient air temperature according to the yearly average value of the location. Results show that by increasing the air temperature, the adsorption capacity decreases, in a more significant way for metal organic frameworks compared to amine functionalized sorbents. An opposite effect is for energy consumption. Moreover, by increasing the ambient air temperature, a higher environmental impact (in terms of climate change) is present. A trend with the air temperature was not found for total costs. Overall, locations with lower ambient air temperatures are preferred due to a lower environmental impact and energy consumption.
High M, Patzschke C, Zheng L, et al., 2022, Hydrotalcite-derived copper-based oxygen carrier materials for efficient chemical-looping combustion of solid fuels with CO2 capture, Energy and Fuels, Vol: 36, Pages: 11062-11076, ISSN: 0887-0624
Chemical-looping combustion (CLC) is a promising technology that utilizes metal oxides as oxygen carriers for the combustion of fossil fuels to CO2 and H2O, with CO2 readily sequestrated after the condensation of steam. Thermally stable and reactive metal oxides are desirable as oxygen carrier materials for the CLC processes. Here, we report the performance of Cu-based mixed oxides derived from hydrotalcite (also known as layered double hydroxides) precursors as oxygen carriers for the combustion of solid fuels. Two types of CLC processes were demonstrated, including chemical looping oxygen uncoupling (CLOU) and in situ gasification (iG-CLC) in the presence of steam. The Cu-based oxygen carriers showed high performance for the combustion of two solid fuels (a lignite and a bituminous coal), maintaining high thermal stability, fast reaction kinetics, and reversible oxygen release and storage over multiple redox cycles. Slight deactivation and sintering of the oxygen carrier occurred after redox cycles at an very high operation temperature of 985 °C. We expect that our material design strategy will inspire the development of better oxygen carrier materials for a variety of chemical looping processes for the clean conversion of fossil fuels with efficient CO2 capture.
High M, Patzschke C, Zheng L, et al., 2022, Precursor engineering of hydrotalcite-derived redox sorbents for reversible and stable thermochemical oxygen storage, Nature Communications, Vol: 13, ISSN: 2041-1723
Chemical looping processes based on multiple-step reduction and oxidation of metal oxideshold great promise for a variety of energy applications, such as CO2 capture and conversion, gasseparation, energy storage, and redox catalytic processes. Copper-based mixed oxides are one of themost promising candidate materials with a high oxygen storage capacity. However, the structuraldeterioration and sintering at high temperatures is one key scientific challenge. Herein, we report aprecursor engineering approach to prepare durable copper-based redox sorbents for use inthermochemical looping processes for combustion and gas purification. Calcination of the CuMgAlhydrotalcite precursors formed mixed metal oxides consisting of CuO nanoparticles dispersed in the MgAl oxide support which inhibits the formation of copper aluminates during redox cycling. The copperbased redox sorbents demonstrated enhanced reaction rates, stable O2 storage capacity over 500 redoxcycles at 900 °C, and efficient gas purification over a broad temperature range. We expect that ourmaterials design strategy has broad implications on synthesis and engineering of mixed metal oxides fora range of thermochemical processes and redox catalytic applications.
Leonzio G, Fennell PS, Shah N, 2022, Analysis of technologies for carbon dioxide capture from the air, Applied Sciences-Basel, Vol: 12, ISSN: 2076-3417
Hennequin LM, Kim S, Monroe EA, et al., 2022, Reclamation of nutrients, carbon, and metals from compromised surface waters fated to the Salton Sea: Biomass production and ecosystem services using an attached periphytic algae flow-way, ALGAL RESEARCH-BIOMASS BIOFUELS AND BIOPRODUCTS, Vol: 66, ISSN: 2211-9264
Ghaedi H, Kalhor P, Zhao M, et al., 2022, Potassium carbonate-based ternary transition temperature mixture (deep eutectic analogues) for CO<sub>2</sub> absorption: Characterizations and DFT analysis, FRONTIERS OF ENVIRONMENTAL SCIENCE & ENGINEERING, Vol: 16, ISSN: 2095-2201
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- Citations: 5
Meka W, Szuhanszki J, Finnry K, et al., 2022, Modeling and Evaluation of Ash-Forming Element Fate and Occurrence in Woody Biomass Combustion in an Entrained-Flow Burner, ACS OMEGA, Vol: 7, Pages: 16306-16322, ISSN: 2470-1343
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- Citations: 1
Leonzio G, Mwabonje O, Fennell PS, et al., 2022, Environmental performance of different sorbents used for direct air capture, Sustainable Production and Consumption, Vol: 32, Pages: 101-111, ISSN: 2352-5509
Currently, conventional carbon dioxide (CO2) mitigation solutions may be insufficient to achieve the stringent environmental targets set for the coming decades. CO2 removal (CDR) technologies, such as direct air capture (DAC), capturing CO2 from the ambient air, are required.In this research, an independent life cycle assessment (LCA) of DAC adsorption systems based on three physisorbents (metal organic frameworks) and two chemisorbents (amine functionalized sorbents) is presented. These capture processes have been optimised by us in previous work.Results show that for the overall capture process, negative CO2 emissions are ensured by using a cellulose-based amine sorbent (cradle-to-gate) ensuring even the net removal of CO2 from the atmosphere (cradle-to-grave). Processes using physisorbents have poorer performances. Chemisorbents yield operating conditions allowing lower impacts on the environment. In 2050, these processes could reduce climate change but can generate other environmental impacts.With the aim to have better environmental performances of DAC systems, future research should be focused on improving the physical properties of sorbents such as the silica gel based amine sorbent to increase their capture capacities. If metal organic frameworks are to be used, it is necessary to drop their energy consumption (by increasing the loading) and the required mass of sorbent.
Fennell P, Driver J, Bataille C, et al., 2022, Going net zero for cement and steel, NATURE, Vol: 603, Pages: 574-577, ISSN: 0028-0836
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- Citations: 31
Bahzad H, Fennell P, Shah N, et al., 2022, Techno-economic assessment for a pumped thermal energy storage integrated with open cycle gas turbine and chemical looping technology, Energy Conversion and Management, Vol: 255, Pages: 1-23, ISSN: 0196-8904
Pumped thermal energy storage offers a high energy density, potentially resulting in a relatively low cost per unit of energy stored. In this study, two novel energy storage systems were developed. The first system was developed by integrating pumped thermal energy storage and chemical looping technologies, whereas the second was formed by merging the first system with an open cycle gas turbine. Both systems used an oxygen depleted stream as a working fluid and iron-based oxygen carriers from a chemical looping water splitting process storage material for the pumped thermal energy storage system. In addition, hydrogen from the chemical looping process was employed for the gas turbine in the second system. Both systems were evaluated thermodynamically via the determination of the roundtrip efficiency. The results presented here indicate that the roundtrip efficiency of both systems developed was 77%. Furthermore, the capital requirements, operating costs, and daily profits from electricity generation were calculated for both systems over several days within the year. The capital and operating costs for the several days that were simulated for the integrated pumped thermal energy storage system were lower than that of a gas turbine based system. Consequently, the daily profit was estimated and found to be between 4.9% and 72.9% higher for the integrated pumped storage relative to the gas turbine based system. Moreover, an economic sensitivity analysis was performed to identify the factors that strongly affect the daily profits of the gas turbine system relative to the pumped storage system. Based on the analysis, the optimal hydrogen fuel percentage fed to the open cycle gas turbine was calculated for the days simulated. Finally, the impact of % error on the estimated capital and fuel production costs on daily profits were investigated. The outcome revealed a higher impact of computational errors on the fuel costs relative to the costs of the capital.
Leonzio G, Fennell PS, Shah N, 2022, A comparative study of different sorbents in the context of direct air capture (DAC): evaluation of key performance indicators and comparisons, Applied Sciences-Basel, Vol: 12, ISSN: 2076-3417
Direct air capture can be based on an adsorption system, and the used sorbent (chemisorbents or physisorbents) influences process. In this work, two amine-functionalized sorbents, as chemisorbents, and three different metal organic frameworks, as physisorbents, are considered and compared in terms of some key performance indicators. This was carried out by developing a mathematical model describing the adsorption and desorption stages. An independent analysis was carried out in order to verify data reported in the literature. Results show that the equilibrium loading is a critical parameter for adsorption capacity, energy consumption, and cost. The considered metal organic frameworks are characterized by a lower equilibrium loading (10−4 mol/kg) compared to chemisorbents (10−1 mol/kg). For this reason, physisorbents have higher overall energy consumptions and costs, while capturing a lower amount of carbon dioxide. A reasonable agreement is found on the basis of the operating conditions of the Climeworks company, modelling the use of the same amine cellulose-based sorbent. The same order of magnitude is found for total costs (751 USD/tonneCO2 for our analysis, compared to the value of 600 USD/tonneCO2 proposed by this company)
Chambon CL, Verdía P, Fennell PS, et al., 2021, Process intensification of the ionoSolv pretreatment: effects of biomass loading, particle size and scale-up from 10 mL to 1 L, Scientific Reports, Vol: 11, Pages: 1-15, ISSN: 2045-2322
The ionoSolv process is one of the most promising technologies for biomass pretreatment in a biorefinery context. In order to evaluate the transition of the ionoSolv pretreatment of biomass from bench-scale experiments to commercial scale, there is a need to get better insight in process intensification. In this work, the effects of biomass loading, particle size, pulp washing protocols and 100-fold scale up for the pretreatment of the grassy biomass Miscanthus giganteus with the IL triethylammonium hydrogen sulfate, [TEA][HSO4], are presented as a necessary step in that direction. At the bench scale, increasing biomass loading from 10 to 50 wt% reduced glucose yields from 68 to 23% due to re-precipitation of lignin onto the pulp surface. Omitting the pulp air-drying step maintained saccharification yields at 66% at 50 wt% loading due to reduced fiber hornification. 100-fold scale-up (from 10 mL to 1 L) improved the efficacy of ionoSolv pretreatment and increasing loadings from 10 to 20 wt% reduced lignin reprecipitation and led to higher glucose yields due to the improved heat and mass transfer caused by efficient slurry mixing in the reactor. Pretreatment of particle sizes of 1–3 mm was more effective than fine powders (0.18–0.85 mm) giving higher glucose yields due to reduced surface area available for lignin re-precipitation while reducing grinding energy needs. Stirred ionoSolv pretreatment showed great potential for industrialization and further process intensification after optimization of the pretreatment conditions (temperature, residence time, stirring speed), particle size and biomass loading. Pulp washing protocols need further improvement to reduce the incidence of lignin precipitation and the water requirements of lignin washing.
Hennequin LM, Tan S-Y, Jensen E, et al., 2021, Combining phytoremediation and biorefinery: Metal extraction from lead contaminated Miscanthus during pretreatment using the ionoSolv process, INDUSTRIAL CROPS AND PRODUCTS, Vol: 176, ISSN: 0926-6690
Eschenbacher A, Fennell P, Jensen AD, 2021, A Review of Recent Research on Catalytic Biomass Pyrolysis and Low-Pressure Hydropyrolysis, ENERGY & FUELS, Vol: 35, Pages: 18333-18369, ISSN: 0887-0624
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- Citations: 9
Fennell PS, Davis SJ, Mohammed A, 2021, Decarbonizing cement production, JOULE, Vol: 5, Pages: 1305-1311, ISSN: 2542-4351
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- Citations: 46
Hennequin L, Sas E, Frémont A, et al., 2021, Biorefinery potential of sustainable municipal wastewater treatment using fast-growing willow, Science of the Total Environment, ISSN: 0048-9697
Hallett J, 2021, Rhododendron and Japanese Knotweed: invasive species as innovative crops for second generation biofuels, RSC Advances: an international journal to further the chemical sciences, Vol: 11, Pages: 18395-18403, ISSN: 2046-2069
We investigated the potential of two terrestrial biomass invasive species in the United-Kingdom as lignocellulosic biofuel feedstocks: Japanese Knotweed (Fallopia japonica) and Rhododendron (Rhododendron ponticum). We demonstrate that a pretreatment technique using a low-cost protic ionic liquid, the ionoSolv process, can be used for such types of plant species considered as waste, to allow their integration into a biorefinery. N,N,N-Dimethylbutylammonium hydrogen sulfate ([DMBA][HSO4]) was able to fractionate the biomass into a cellulose-rich pulp and a lignin stream at high temperatures (150–170 °C) and short reaction times (15–60 minutes). More than 70–80% of the subsequent cellulose was hydrolysed into fermentable sugars, which were fermented into the renewable energy vector bioethanol.
Yao JG, Tan S-Y, Metcalfe P, et al., 2021, Demetallization of Sewage Sludge Using Low-Cost Ionic Liquids, ENVIRONMENTAL SCIENCE & TECHNOLOGY, Vol: 55, Pages: 5291-5300, ISSN: 0013-936X
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- Citations: 11
Patzschke CF, Boot-Handford ME, Song Q, et al., 2021, Co-precipitated Cu-Mn mixed metal oxides as oxygen carriers for chemical looping processes, Chemical Engineering Journal, Vol: 407, Pages: 1-14, ISSN: 1385-8947
Chemical looping with oxygen uncoupling (CLOU) and chemical looping air separation (CLAS) are novel and potentially promising processes for the combustion of solid fuels (e.g. biomass) for power generation with inherent CO2 capture. Redox-experiments at 850–950 °C confirmed that copper manganese spinel oxides are promising oxygen carriers for these processes, as they combine a relatively high O2 release capacity and fast O2 release kinetics. Furthermore, this work presents a novel method to calculate the O2 partial pressure equilibrium and the heat of O2 release from observed rates of reaction. To demonstrate this method, oxygen carriers were prepared via mechanical mixing and co-precipitation with varying molar Cu:Mn ratios and synthesis conditions, thereby tuning material properties and the pore structure. The precursors and calcined materials were characterised, and the crystalline phases were determined using X-ray diffraction. The insights from the post cycling analysis of the oxygen carriers and the experimentally obtained O2 release capacities were combined to elucidate the redox-reactions relevant for the two processes. It was found that the presence of a higher partial pressure of O2 during the O2 release results in the formation of different (perovskite-like) phases than those occurring during the decomposition in an O2-free environment. The oxygen carriers demonstrated excellent stability at CLOU and CLAS process conditions during extended redox cycling (100 cycles in a thermo-gravimetric analyser and 50 cycles in a fluidised bed reactor), showing no significant loss of reactivity or O2 release capacity and a high resistance towards attrition and agglomeration. The degree of degradation after 100 cycles was in the order: temperature swing (CLAS) < O2 partial pressure swing (CLOU) < reduction with CH4 (chemical looping combustion).
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