Enhanced CO₂ Conversion to CO by Silica-Supported Perovskite Oxides at Low Temperatures

摘要

Repurposing of CO_(2) to valuable hydrocarbons is crucial for energy security and a balanced carbon cycle. Reverse water gas shift chemical looping (RWGS-CL) is capable of efficient CO_(2) to CO conversion at a low temperature of ～600 °C with unprecedented rates using the La_(0.75)Sr_(0.25)FeO_(3) (LSF) perovskite-type oxide amalgamated with silica. The LSF/SiO_(2) composite (25% LSF by mass) promotes a notable extent of oxygen vacancies in the active phase, a key parameter for CO_(2) conversion. In each of eight RWGS-CL cycles, CO generation yields of LSF/SiO_(2) surpass those of LSF alone by about 200%, producing 2.6 mmol of CO g_(LSF)~(–1) at a peak rate of 0.8 mmol CO g_(LSF)~(–1) min~(–1). This significant improvement is concomitant with a decreased average LSF crystallite size retained at these low thermochemical reaction temperatures. Evidence of this enhancement points to perovskite particle size reduction by silica, lattice strain induced by the support, and curtailed quantities of secondary phases that limit accessibility to active surfaces. In this contribution, an appropriate stable platform for improving earth abundancy in perovskite-based redox materials is demonstrated for industrial-scale low-temperature CO_(2) thermochemical conversion.