Pre-combustion packed bed chemical looping (PCCL) technology for efficient H2-rich gas production processes

• A novel process based on chemical looping for H2/N2 syngas production has been presented.
• The experimental proof of principle has been carried out in a 2 kW packed bed reactor.
• A Fe-based OC has been tested in the range 600–800 °C.
• The PCCL system has an electrical efficiency up to 51.5%.

A novel reactor system is presented and investigated for the production of a hydrogen rich gas stream for power or ammonia production, based on pre-combustion chemical looping (PCCL) technology using dynamically operated packed bed reactors. In this process, the oxygen carrier (OC) is alternately oxidized with a gas mixture of air and steam to produce a H2/N2 product gas stream combining oxidation by air and water-splitting, and subsequently reduced with syngas producing a concentrated CO2 stream. The process is carried out at elevated pressure, but at intermediate temperature (in the range of 600–900 °C), which allows circumventing the extremely high temperatures required in chemical-looping combustion. In addition, the N2/H2 gas stream can be produced at the required composition for ammonia production, rendering this process also competitive with the conventional ammonia production. A preliminary experimental study has been carried out in a 2 kWth packed bed reactor using an iron-based oxygen carrier. The influence of the operating temperature and the initial solid composition during the oxidation cycle on the H2-rich gas yield has been investigated. The complete reduction to pure iron reduces the reactivity of the material due to sintering, whereas a controlled reduction to wüstite (FeO) allows to maintain a higher stability of the material, although the oxygen capacity is decreased.A preliminary thermodynamic assessment of the integrated PCCL plant for power production with natural gas has been carried out reaching an electrical efficiency of 49–51.5% (depending on the plant arrangement) with a carbon capture rate above 95%. The main parameter affecting the plant performance was found to be the steam requirement during the oxidation cycle. The comparison with benchmark technologies has confirmed the potential of the PCCL system.

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