Recovery of N2O: Energy-Efficient and Structure-Driven Clathrate-Based Greenhouse Gas Separation

초록

N2O has 300 times more global warming potential than CO2 and is also one of the main stratospheric ozone-depleting substances emitted by human activities such as agriculture, industry, and the combustion of fossil fuels and solid waste. We present here an energy-efficient clathrate-based greenhouse gas-separation (CBGS) technology that can operate at room temperature for selectively recovering N2O from gas mixtures. Clathrate formation between alpha-form/beta-form hydroquinone (alpha-HQ/beta-HQ) and gas mixtures reveals guest-specific and structuredriven selectivity, revealing the preferential capture of N2O in beta HQ and the molecular sieving characteristics of alpha-HQ. With a maximum gas storage capacity and cage occupancy of 54.1 cm(3) g(-1) and 0.86, respectively, HQ clathrate compounds including N2O are stable at room temperature and atmospheric pressure and thus can be easily synthesized, treated, and recycled via commercial CBGS processes. High selectivity for N2O recovery was observed during beta-HQ clathrate formation from N2O/N-2 gas mixtures with N2O concentrations exceeding 20%, whereas alpha-HQ traps only N-2 molecules from gas mixtures. Full characterization using X-ray diffraction, scanning electron microscopy, Raman spectroscopy, solid-state nuclear magnetic resonance, and compositional analysis and the formation kinetics of HQ clathrates was conducted to verify the peculiar selectivity behavior and to design the conceptual CBGS process. These results provide a new playground on which to tailor host-guest materials and develop commercial processes for the recovery and/or sequestration of greenhouse gases.

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