Performance evaluation of novel Ca/Mn-doped perovskite as a multifunctional material in chemical looping reverse water gas shift process for low-carbon fuels

Abstract

The chemical looping reverse water gas shift (CL-RWGS) catalytic process offers a promising approach for decarbonizing energy-intensive industries. The CL-RWGS promotes the formation of surface oxygen vacancies in the material, which are subsequently replenished by extracting oxygen from CO2, resulting in syngas production. However, there remains a significant gap in the development of materials that not only exhibit redox activity but also enable in-situ carbonation, offering dual functionality for enhanced CO2 utilization. This study introduces a
novel calcium- and manganese-doped LaNiO3 perovskite, designed for integrated CO2 sorption and in-situ utilization during CL–RWGS process. Comprehensive characterization confirmed the material’s crystalline structure, porosity, and successful incorporation of Ca and Mn dopants. Thermogravimetric analysis (TGA) across 700 – 900 ◦C revealed a peak oxygen storage capacity of 1.97 mmol O2/g and demonstrated excellent redox stability, with less than 1 % performance loss over 17 cycles. RWGS experiments conducted in a packed bed reactor demonstrated up to 57 % CO2 to CO conversion at 900 ◦C, approaching the thermodynamic equilibrium value of 60 % under the same operating conditions. Moreover, an H2/CO molar ratio of ~2.0, suitable for Fischer-Tropsch
synthesis, was achieved at 600 ◦C and 1.0 bar with a feed H2/CO2 molar ratio of 1.0, attributed to CO2 chemisorption via a carbonation-driven mechanism facilitated by the presence of CaO phase. These results suggest that the calcium- and manganese-doped LaNiO3 perovskite is a highly promising multi-functional material for chemical looping-based CO2 utilization technologies.

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Identifiers

ORCID for Syed Zaheer Abbas: orcid.org/0000-0002-8783-8572

ORCID for Mohamed G Hassan: orcid.org/0000-0003-3729-4543

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