An excessive amount of CO2 is the leading cause of climate change, and hence, its reduction in the Earth's atmosphere is critical to stop further degradation of the environment. Although a large body of work has been carried out for post-combustion low-temperature CO2 capture, there are very few high temperature pre-combustion CO2 capture processes. Lithium silicate (Li4SiO4), one of the best known high-temperature CO2 capture sorbents, has two main challenges, moderate capture kinetics and poor sorbent stability. In this work, we have designed and synthesized lithium silicate nanosheets (LSNs), which showed high CO2 capture capacity (35.3 wt% CO2 capture using 60% CO2 feed gas, close to the theoretical value) with ultra-fast kinetics and enhanced stability at 650 degrees C. Due to the nanosheet morphology of the LSNs, they provided a good external surface for CO2 adsorption at every Li-site, yielding excellent CO2 capture capacity. The nanosheet morphology of the LSNs allowed efficient CO2 diffusion to ensure reaction with the entire sheet as well as providing extremely fast CO2 capture kinetics (0.22 g g(-1) min(-1)). Conventional lithium silicates are known to rapidly lose their capture capacity and kinetics within the first few cycles due to thick carbonate shell formation and also due to the sintering of sorbent particles; however, the LSNs were stable for at least 200 cycles without any loss in their capture capacity or kinetics. The LSNs neither formed a carbonate shell nor underwent sintering, allowing efficient adsorption-desorption cycling. We also proposed a new mechanism, a mixed-phase model, to explain the unique CO2 capture behavior of the LSNs, using detailed (i) kinetics experiments for both adsorption and desorption steps, (ii) in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy measurements, (iii) depth-profiling X-ray photoelectron spectroscopy (XPS) of the sorbent after CO2 capture and (iv) theoretical investigation through systematic electronic structure calculations within the framework of density functional theory (DFT) formalism.

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