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Potassium and Zeolitic Structure Modified Ultra-microporous Adsorbent Materials from a Renewable Feedstock with Favorable Surface Chemistry for CO2 Capture

Liu, Xin, Sun, Yuan, Liu, Jingjing, Sun, Chenggong, Liu, Hao, Xue, Qian, Smith, Emily, Snape, Colin
ACS Applied Materials & Interfaces 2017 v.9 no.32 pp. 26826-26839
X-ray photoelectron spectroscopy, adsorbents, adsorption, agricultural wastes, carbon, carbon dioxide, carbonization, cations, energy-dispersive X-ray analysis, feedstocks, heat, nanocomposites, porosity, porous media, potassium, rice hulls, silicon compounds, surface area
Novel hierarchically structured microporous biocarbons with exceptionally high capacities for CO₂ capture have been synthesized from the abundant agricultural waste of rice husk (RH), using a facile methodology that effectively integrated carbonization, activation, and potassium intercalation into a one-step process. Textural characterization demonstrates that the synthesized biocarbons exhibit exceedingly high ultra-microporosity accounting for up to 95% of total porosity mainly as a result of the naturally occurring silicon compounds within the RH molecular framework structures. With a modest surface area of up to 1035 m²/g and a total pore volume of 0.43 cm³/g, the best performing RH carbon has shown exceptionally high and fully reversible CO₂ uptake capacity of 2.0 mmol/g at 25 °C and a CO₂ partial pressure of 0.15 bar, which represents one of the highest uptakes ever reported for both carbon and MOF materials usually prepared from using cost-prohibitive precursor materials with cumbersome methodologies. It has been found that up to 50% of the total CO₂ uptake is attributable to the unique surface chemistry of the RH carbons, which appears to be dominated by the enhanced formation of extra-framework potassium cations owing to the exceedingly high levels of ultra-microporosity and the presence of zeolitic structures incorporated within the carbon matrices. Characterizations by EDX element mapping, XPS, and heat of adsorption measurements confirm the existence of a range of zeolitic structures, which essentially transforms the RH carbons into a kind of zeolite–carbon nanocomposite material with strong surface affinity for CO₂.