Biomass chemical looping gasification (BCLG) is emerging as a promising alternative to conventional gasification, addressing inherent limitations. This study systematically compares BCLG with conventional methods like air and air/steam gasification, using pine forest residue in an allothermal fluidized bed reactor. Key operational parameters such as reactor temperature (800–900 °C), equivalence ratio (0.18–0.36) and steam-to-biomass ratio (1.3) were examined. Performance indicators such as gas composition, yields, carbon conversion, and cold gas efficiency were evaluated and compared. BCLG without steam displayed similar performance to conventional methods. However, the performance of BCLG with steam surpassed conventional gasification methods and emerged as the most promising process. The results suggest enhanced catalytic performance of nickel smelter slag for reforming reactions under steam-rich conditions, with H₂/CO ratio, product gas yield, cold gas and carbon conversion efficiency improved by approximately 111%, 30%, 14% and 2%, respectively, compared to air/steam gasification.

The study investigates biomass chemical looping gasification (BCLG) using nickel smelter slag as an oxygen carrier (OC). Key operating parameters, including reactor temperatures (800–900 °C), OC-to-biomass ratio (OCBR, 4:1–15:1), and steam as a gasification medium, were evaluated in a 5kW_th fluidized bed reactor using pine forest residue. Performance metrics including gas composition and process efficiencies were assessed. OCs were characterized using XRD, BET and SEM-EDS analyses. Optimal performance was achieved at 850 °C, an OCBR (10:1) and a steam-to-biomass ratio (1.4). The gas composition was 38.87 vol% H₂, 19.65 vol% CO, 34.48 vol% CO₂, and 6.61 vol% CH₄, with a product gas yield of 1.24Nm³/kg-biomass. Carbon conversion efficiency was 77.85 %, cold gas efficiency 58.70 %, and levelized cost of fuel was 0.15 €/Nm³ for product gas and 4.55 €/kg for H₂.The results suggest that steam addition significantly enhanced char conversion, improving overall BCLG efficiency. Moreover, nickel smelter slag demonstrated stability, consistent reactivity, and limited sintering behavior.

Biomass Chemical Looping Gasification (BCLG) is a cost-effective and efficient alternative to conventional gasification. The selection of appropriate oxygen carriers (OCs) is crucial for stable BCLG performance. These OCs need to possess high reactivity, selectivity, material strength, and resistance to sintering. The study investigated various OC materials, including industrial wastes (copper, nickel slag, desulphurization, LD, and ladle slags), residential waste (sewage sludge ash), and natural ore (manganese). The evaluation of OCs focused on reactivity, H₂-selectivity, mechanical strength and sintering behaviour. Except for ladle slag, all OC samples exhibited favourable reactivity due to the presence of Fe- and Mn-oxides possessing high oxygen transport capacity (10–17.6%). Nickel slag, manganese ore, and desulphurisation slag displayed notable H₂-selectivity (8.7 to 10.4). It can be attributed to the presence of less-active (lattice) oxygen, limiting strong oxygen agents such as Fe₂O₃, Fe₃O₄, and Mn₂O₃. Moreover, desulphurization slag contained highly selective Ca₂Fe₂O₅, which falls within the partial oxidation zone of the Ellingham diagram. Furthermore, all OC samples exhibited desirable material strength (>20 MPa), suitable for fluidised bed reactors. However, nickel, LD, and ladle slags demonstrated limited sintering with sintering onset temperatures exceeding 963 °C. This limited sintering may be attributed to the absence of iron silicates, iron-bearing aluminium silicates, manganese silicates, and potassium that contributed to the low thermal stability observed in the remaining OCs. Altogether, nickel slag calcined at 1100 °C was identified as the most promising OC material with optimal reactivity, selectivity, material strength, and minimal sintering for BCLG. Overall, this study provides a detailed and scientific methodology for OC selection and can aid future OC development.

Biomass chemical looping gasification (BCLG) offers significant advantages over the conventional biomass gasification process in terms of enhanced gasification efficiency, inherent CO₂ capture, process circularity, and mitigated emissions of pollutants. This review discusses the prevailing status of research and development of BCLG in terms of production of high-quality syngas and negative carbon emissions based on the latest experimental and modelling studies. In particular, the design of the BCLG process and reactors is compared with conventional gasification. This review suggests that the BCLG process could be 10–25 % more efficient than the conventional combustion and gasification system in terms of economical H₂-production cost (3.37 USD/kg H₂-produced) and negative life cycle emissions of CO₂ (−14.58 kg-CO₂e/ kg-H₂ produced). This review has extensively considered the effects of process parameters and oxygen carriers (OCs) on gasification chemistry and reaction engineering during BCLG experiments. More specifically, the properties of OCs have been holistically analysed from technological, economic, and environmental perspectives to screen appropriate and affordable OCs for BCLG. In addition, the state-of-the-art modelling studies on BCLG are compared in terms of thermodynamic equilibrium, kinetics, and integrated processes. Technological challenges and research gaps in experiments and modelling have been highlighted in order to advance the BCLG process for industrial applications. In particular, further experimental work is needed to tackle issues related to stability and deactivation of OCs, fluidisation and circulation, the mechanical strength of OCs, the optimisation of feed conversion, and the integration and management of various thermal reactors. It is also desired to enhance the accuracy of models by incorporating optimisation of integrated processes and a more detailed reaction mechanism. Overall, BCLG is a promising negative emissions technology for renewable energy production, yet more innovative efforts in experimental and modelling studies are imperative to move towards more practical applications.

Globally, large amounts of biomass wastes such as cattle manure, fruit/vegetable waste, and cheese whey residual streams are disposed of from farming and food processing industries. A promising approach to convert such biogenic residues into valuable biofuels is Supercritical Water Gasification (SCWG). A detailed investigation on SCWG of the mentioned wet biomass wastes has been performed to assess the thermodynamic behavior of such a complicated system. This is conducted by combining advanced models with a supplementary experimental study, providing deep insight into the behavior of the SCWG system for different bio-waste sources. For the modelling part, different approaches including global, constrained and thermal quasi-thermodynamic equilibria have been pursued to analyze the influence of operating parameters on the produced biogas quality. Furthermore, SCWG experiments were conducted using biomass samples provided by our industrial partner. Reasonable agreements were observed between experimental results and predictions from constrained and thermal-quasi equilibrium models, showing significant improvements over the global thermodynamic equilibrium model. Results showed that superimposition of carbon conversion efficiency together with the use of a constant molar amount of specific compounds can improve the accuracy of the global equilibrium model. Furthermore, comparisons between different models revealed the advantage of the thermal quasi-equilibrium model, which uses the “approach temperature” concept, over the constrained equilibrium model, by reducing the complexities inherent in superimposing multiple constraints. Overall, the thermal-quasi equilibrium approach has its advantages of lumping all the additional constraints used in the constrained equilibrium model into an effective approach temperature, offering (i) a better reproducibility of the experimental data point and (ii) a rigorous basis for scale-up calculation. The results of this study provide a better understanding of the SCWG process for different types of wet biomass feedstocks as result of applying advanced analytical approaches and comparing with experiments.

We investigate forced convective heat transfer in packings of spheres, cylinders and Raschig rings, made of glass, steel and alumina, in relatively narrow tubes. A detailed comparison is made between resolved pellet-scale, azimuthally-averaged temperature profiles, and 2D-axially-dispersed pseudo-homogenous plug flow (2D-ADPF) predictions. The local temperature deviates significantly from azimuthally-averaged profiles, which in turn deviate from 2D-ADPF predictions. We show that the length dependency of effective heat transfer parameters is caused by thermal (non-)equilibrium between fluid and solid phases along the bed and not related to inadequate insulation of the calming section or the thermocouple's cross or an under-developed velocity and thermal field at the bed inlet. The influence of pellet shape and thermal conductivity and tube-to-pellet diameter ratio on k_er and h_w are assessed. We conclude that the models of Specchia/Baldi/Gianetto/Sicardi for all flow regimes and of Martin/Nilles for the turbulent regime are recommended for practical use for spherical particles.

This paper investigates the validity of azimuthal averaging of 3D temperature fields in the analysis of lateral heat transfer in dense particle packings. This is conducted by synthetic generation of 3D packing surrogates of spheres, cylinders and Raschig rings with tube-to-pellet diameter ratio, 3 < N < 6, using an in-house Rigid Body Dynamics packing algorithm, followed by detailed discrete pellet CFD simulations of heat transfer from wall to bed for laminar, transient and turbulent flow regimes. The CFD results of hydrodynamics and temperature fields are benchmarked against empirical correlations for pressure drop and interphase heat transfer Nusselt number, Nu, offering the best fits with correlations proposed by Eisfeld and Schnitzlein (for cylinders and spheres) and Nemec and Levec (for rings) for pressure drop, and by Gunn and Sun and coworkers for the prediction of Nu. The CFD results demonstrate that fluctuations in local temperature are completely neglected by azimuthal-averaging of 3D temperature fields over the bed volume, leading to more than 150 °C deviations from the local temperature data. Furthermore, it is found that deviations between azimuthally-averaged axial velocity profile and true local velocities are in an analogous fashion transmitted to the temperature field. This is evidenced by the coincidence of the peaks in the deviation profiles of azimuthally-averaged temperature and velocity from the local data over the bed radius. This is due to thermal disequilibrium between fluid and pellet phases which is partially omitted by the azimuthal-averaging of the 3D temperature field and basically neglected in pseudo-homogenous k_er-h_w models.

The local flow structure and pressure drop in random packings of Raschig rings are analyzed using sequential Rigid Body Dynamics (RBD) method and Computational Fluid Dynamics (CFD) simulation. Tube-to-pellet diameter ratios, N, between 3 and 6 are investigated for laminar, transitional and turbulent flow regimes (5 ≤ Re_p ≤ 3,000). The computed pressure drops are in good agreement with the empirical correlation of Nemec and Levec (2005), while the Ergun equation exhibited high deviations of more than 60%, even when it is modified to explicitly account for non-sphericity of pellets. This deviation is ascribed to additional sources for eddy formation offered by Rashig rings, compared to spheres and cylinders, which cannot be counterbalanced by the usage of a higher specific surface area. The 3D results of flow structure demonstrate a large influence of packing topology on the velocity distribution: rings oriented parallel to the flow accelerate the local velocity through their axial holes, while rings oriented perpendicular to the flow provide additional space for vortex formation. The flow fields are substantially different from that found in packings of spheres and cylinders, both in terms of volume of backflow regions and velocity hotspots. This implies a higher order of local flow inhomogeneity in azimuthal and axial directions compared to spherical and cylindrical packings. Furthermore, it is found that azimuthal averaging of the 3D velocity field over the bed volume, which has been used to improve classical plug-flow pseudo-homogenous models to account for the role of tortuous velocity fields, cannot reflect the appearance of vortex regions and thereby leads to underestimation of the local axial velocity values by over 500% of the inlet velocity.

Despite the substantial simplicities inherent in pseudo-continuum models of fixed bed reactors, there is a continued interest in the use of such models for predicting fluid flow and transport scalars. In this paper, we aim to quantitatively address the inadequacy of 2D pseudo-continuum models for narrow-tube fixed beds. We show this by comparing with spatially resolved 3D results obtained by a robust and integrated numerical workflow, consisting of a sequential Rigid Body Dynamics and Computational Fluid Dynamics (RBD-CFD) approach. The RBD is founded on a physics-based hard-body packing algorithm, recently proposed by the authors (Moghaddam, E.M., Foumeny, E.A., Stankiewicz, A.I., Padding, J.T., 2018. A Rigid Body Dynamics Algorithm for Modelling Random Packing Structures of Non-Spherical and Non-Convex Pellets. Ind. Eng. Chem. Res. 57, 14988–15007), which offers a rigorous method to handle resting contacts between particles. The methodology is benchmarked for simulations of flow fields in all flow regimes, for 5 ≤ Re_p ≤ 3,000, in random packings of spheres and cylinders with tube-to-pellet diameter ratios, N, between 2.29 and 6.1. The CFD results reveal a remarkable influence of local structure on the velocity distribution at the pellet scale, particularly in low-N packings, where the spatial heterogeneity of the structure is very strong along the bed axis. It is also demonstrated that azimuthal averaging of the 3D velocity field over the bed volume, which has been considered as an advancement over plug flow idealization in classical pseudo-continuum models, cannot reflect the role of vortex regions emerging in the wake of the pellets, and leads to underestimation of the local velocity values by more than 400% of the inlet velocity.

Despite the common use of nonspherical catalyst pellets in chemical engineering applications, the packing structures of such pellets have not been as systematically studied and characterized as spherical packings. We propose a packing algorithm based on rigid body dynamics to simulate packing of nonspherical and possibly nonconvex pellets. The algorithm exerts a hard-body approach to model collision phenomena. The novelty is that the transition between moving and resting particles is controlled by a cutoff on the relative contact velocities, instead of artificially damping linear and angular velocities to stabilize the algorithm. The algorithm is used to synthesize packings of spheres, cylinders, and Raschig rings with tube-to-pellet diameter ratios 3-9.16. The packings are validated in terms of bulk porosity and radial void fraction distribution, finding satisfactory agreement with literature data. Denser packing structures are generated with high restitution coefficients and low friction coefficients. The confining tube walls play an important role, with highly fluctuating bulk porosities in narrow tubes.