Efficient in situ conversion of captured CO₂ into fuels enabled by direct solar driven multifunctional calcium looping

Carbon neutrality requires credible action to reduce greenhouse gas emissions and develop clean and renewable energy. The solar driven multifunctional calcium looping (CaL), which integrates CO₂ capture, CO₂ conversion into fuels, and thermochemical energy storage into a solar driven cycle, tends to be one of the most promising pathways to establish a zero-carbon energy system. However, the progress of this concept remains in the proof-of-principle stage and the research into its magnified operations and underlying fundamental scientific problems is seldom reported. In fact, the thermodynamic and kinetic features of this integrated cycle are intertwined during the solar harvesting, CO₂ capture, calcination, and CO₂ reduction processes, so that the synergetic manipulation of the reactions becomes vital and challenging. Here, attempts are made to develop the design and regulation scheme for implementing full-scale application according to the research into a preliminarily enlarged operation carried out in a stirred bed reaction system. The kinetic matching relationships between different chemical reactions involving intense heat and mass transfer across the entire solar energy conversion chain are investigated. The average solar absorption of CaCO₃ based composite particle material is promoted to 90.9% through doping catalysts into CaCO₃. The solar-to-chemical conversion efficiency reaches up to 51.6%. More than 88.2% of the CO₂ is converted into syngas in-situ. The high energy conversion efficiency indicates the bright prospect of such a direct solar driven multifunctional CaL system, and the proposed design and enhancement methods are expected to provide theoretical and practical references for its industrialization process.