Chemical looping gasification (CLG) is a novel gasification technique, allowing for the production of a nitrogen-free high calorific synthesis gas from solid hydrocarbon feedstocks, without requiring a costly air separation unit. Initial advances to better understand the CLG technology were made during first studies in lab and bench scale units and through basic process simulations. Yet, tailored process control strategies are required for larger CLG units, which are not equipped with auxiliary heating. Here, it becomes a demanding task to achieve autothermal CLG operation, for which stable reactor temperatures are obtained. This study presents two avenues to attain autothermal CLG behavior, established through equilibrium based process simulations. As a first approach, the dilution of active oxygen carrier materials with inert heat carriers to limit oxygen transport to the fuel reactor has been investigated. Secondly, the suitability of restricting the air flow to the air reactor in order to control the oxygen availability in the fuel reactor was examined. Process simulations show that both process control approaches facilitate controlled and de-coupled heat and oxygen transport between the two reactors of the chemical looping gasifier, thus allowing for efficient autothermal CLG operation. With the aim of inferring general guidelines on how CLG units have to be operated in order to achieve decent synthesis gas yields, different advantages and disadvantages associated to the two suggested process control strategies are discussed in detail and optimization avenues are presented.

Chemical looping gasification (CLG) is a promising process for the thermochemical solid to liquid conversion route using lattice oxygen, provided by a solid oxygen carrier material, to produce a nitrogen free synthesis gas. Recent advances in lab-scale experiments show that CLG with biomass has the possibility to produce a carbon neutral synthesis gas. However, all experiments have been conducted in externally heated units, not enabling autothermal operation. In this study, the modification of an existing pilot plant for demonstrating autothermal operation of CLG is described. Energy and mass balances are calculated using a validated chemical looping combustion process model extended for biomass gasification. Based on six operational cases, adaptations of the pilot plant are designed and changes discussed. A reactor configuration using two circulating fluidized bed reactors with internal solid circulation in the air reactor is proposed and a suitable operating strategy devised. The resulting experimental unit enables a reasonable range of operational parameters within restrictions imposed from autothermal operation.

Chemical looping gasification (CLG) is a novel dual-fluidized bed gasification technology that allows for the production of high-calorific syngas from various solid feedstocks (e.g., biomass). Solid circulation between the two coupled fluidized bed reactors, serving the purpose of heat and oxygen transport, is a key parameter for the CLG technology, making system hydrodynamics the backbone of the gasification process. This study serves the purpose to provide holistic insights into the hydrodynamic behavior of the dual-fluidized bed reactor system. Here, special focus is placed on the operational principles of the setup as well as the entrainment from the circulating fluidized bed (CFB) reactors, the latter being the driving force for the solid circulation inside the entire reactor system. Using an elaborate dataset of over 130 operating periods from a cold flow model and 70 operating periods from a 1 MW_th CLG pilot plant, a holistic set of ground rules for the operation of the reactor setup is presented. Moreover, a novel easily-applicable approach, solely relying on readily-available live data, is presented and validated using data from the 1 MW_th chemical looping gasifier. Thereby, a straightforward estimation of solid entrainment from any CFB setup is facilitated, thus closing a crucial research gap.