Eikeland Espen, Blichfeld Anders Bank, Tyrsted Christoffer, Jensen Anca, Iversen Bo Brummerstedt
Center for Materials Crystallography, Department of Chemistry and iNANO, Aarhus University , DK-8000 Aarhus C, Denmark.
ACS Appl Mater Interfaces. 2015 Mar 11;7(9):5258-64. doi: 10.1021/am508432w. Epub 2015 Mar 2.
The global ambition of reducing the carbon dioxide emission makes sequestration reactions attractive as an option of storing CO2. One promising environmentally benign technology is based on forming thermodynamically stable carbonated minerals, with the drawback that these reactions usually have low conversion rates. In this work, the carbonation reaction of Mg rich olivine, Mg2SiO4, under supercritical conditions has been studied. The reaction produces MgCO3 at elevated temperature and pressure, with the addition of NaHCO3 and NaCl to improve the reaction rates. A sequestration rate of 70% was achieved within 2 h, using olivine particles of sub-10 μm, whereas 100% conversion was achieved in 4 h. This is one of the fastest complete conversions for this reaction reported to date. The CO2 sequestration rate is found to be highly dependent on the applied temperature and pressure, as well as the addition of NaHCO3. In contrast, adding NaCl was found to have limited effect on the reaction rate. The roles of NaHCO3 and NaCl as catalysts are discussed and especially how their effect changes with increased olivine particle size. The products have been characterized by Rietveld refinement of powder X-ray diffraction, scanning electron microscopy (SEM), and energy-dispersive X-ray (EDX) spectroscopy revealing the formation of amorphous silica and micrometer-sized magnesium carbonate crystals.
减少二氧化碳排放的全球目标使得封存反应作为一种储存二氧化碳的选择颇具吸引力。一种有前景的环境友好型技术基于形成热力学稳定的碳酸化矿物,但其缺点是这些反应通常转化率较低。在这项工作中,研究了富镁橄榄石(Mg₂SiO₄)在超临界条件下的碳酸化反应。该反应在高温高压下生成碳酸镁,并添加碳酸氢钠和氯化钠以提高反应速率。使用粒径小于10μm的橄榄石颗粒,在2小时内实现了70%的封存率,而在4小时内实现了100%的转化率。这是迄今为止报道的该反应最快的完全转化率之一。发现二氧化碳封存率高度依赖于所施加的温度和压力,以及碳酸氢钠的添加。相比之下,发现添加氯化钠对反应速率的影响有限。讨论了碳酸氢钠和氯化钠作为催化剂的作用,特别是它们的效果如何随橄榄石粒径的增加而变化。通过粉末X射线衍射的Rietveld精修、扫描电子显微镜(SEM)和能量色散X射线(EDX)光谱对产物进行了表征,揭示了无定形二氧化硅和微米级碳酸镁晶体的形成。