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Abstract

Biogas-based power-to-X technology allows storing renewable electricity, while producing CO2-neutral products. This work investigates the conversion and upgrading of digestion-derived gas mixtures with focus on increasing the operational flexibility of the overall process. Compensation of fluctuations in the feed gases enable a better economic predictability of the processes and increase the product gas output. A techno-economic evaluation was performed on bubbling fluidised bed (BFB) methanation and biological methanation for CO2 conversion in all-year operation. Each considered process was modelled and optimised to obtain grid-ready biomethane. Rate-based models were used for the main units (BFB reactor, H2-separation membrane). For the biological methanation, simulated performance data from literature were included. The analysis revealed a 17 - 19% lower production cost for BFB methanation, mainly due to lower investment cost for the main reactor vessel. Instead of using PEM electrolysis, high temperature electrolysis (SOE) would allow for heat integration with the BFB reactor, which increases the plant efficiency from 54% to 73% (LHV). A further production cost reduction can be achieved by direct methanation of biogas, omitting prior separation of CO2. Based on gas separation experiments with a commercial biogas upgrading module (Evonik Sepuran) performed in a TRL 5 plant, a flexible upgrading concept using a permeation model was developed. It allows to swiftly switch between conventional membrane-based CO2 separation by a 2-stage membrane unit and direct methanation of biogas and subsequent H2 recycling. A techno-economic analysis was performed on the flexible upgrading concept. The operation hours of the electrolyser were determined by applying a threshold to the electricity price distribution of the past years. The sensitivity on electricity cost (i.e. PtG operation hours) is clearly reduced with the flexible processes, resulting in a better economic predictability of the overall process, compared to a pure PtG installation. System analysis shows the need to allow part load operation of the methanation. Symmetric part load operation (reduced availability of CO2 and H2) was tested in a field experiment by direct methanation of biogas with subsequent H2 recycling in the TRL 5 methanation pilot plant. Stable operation of the methanation plant could be achieved at part load levels from 45% to 100% with closed recycle loop. The BFB reactor alone was tested in a load range of 20 to 100%. A dynamic experiment demonstrated fast, successive load changes while still producing grid-ready biomethane. Asymmetric part load (only H2 limiting) operation was investigated by process simulations and field experiments. Since CO2 is present in the system in an over-stoichiometric amount, H2 recycle and CO2 separation have to be performed simultaneously. Process simulations showed that selecting a most ideal PtG configuration based on technical feasibility is difficult, as further constraints, such as overall economics and operation scheduling have to be considered in process design and evaluation. In all cases, the CO2 separation from the integrated processes leads to a loss of H2 and CH4 from the process. The introduction of an additional membrane stage with a sweep stream is proposed to reduce the loss of reactive gases via the off gas stream.

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