School of Resource and Environmental Sciences, Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, Wuhan University , 430079 Wuhan, China.
Environ Sci Technol. 2016 Oct 4;50(19):10588-10595. doi: 10.1021/acs.est.6b02955. Epub 2016 Sep 16.
Efficient and high-flux capture of CO is the prerequisite of its utilization. Static absorption of CO with solid LiO and molten salts (LiO-free and LiO-containing Li-Na-K carbonates) was investigated using a reactor with in situ pressure monitoring. The absorption capacity of dissolved LiO was 0.835 mol/mol at 723 K, larger than that of solid LiO. For the solid LiO absorbents, formation of solid LiCO on the surface can retard the further reactions between LiO and CO, whereas the dissociation/dissolution effect of molten carbonate on LiO improved the mass-specific absorption capacity of liquid LiO. In LiO-containing Li-Na-K molten carbonate, CO was mostly absorbed by alkaline oxide ions (O). The chemical interactions between CO and CO contributed to CO uptake via formation of multiple carbonate ions. The mass transfer of these absorbing ions was found as the dominating factor governing the rate of static absorption. Higher temperatures reduced the thermodynamic tendency of CO absorption, but a lower viscosity at elevated temperature was conducive to absorption kinetics. Compared with the commonly used CaO absorbent, LiO was much more dissolvable in molten carbonate. The LiO-containing molten carbonate is potentially a promising medium for industrial carbon capture and electrochemical transformation process.
高效、高通量地捕获 CO 是其利用的前提条件。采用具有原位压力监测功能的反应器,研究了 CO 与固体 LiO 和熔融盐(无 LiO 和含 LiO 的 Li-Na-K 碳酸盐)的静态吸收。在 723 K 时,溶解 LiO 的吸收容量为 0.835 mol/mol,大于固体 LiO 的吸收容量。对于固体 LiO 吸收剂,表面上形成的固体 LiCO 可以阻止 LiO 与 CO 之间的进一步反应,而熔融碳酸盐对 LiO 的解离/溶解作用提高了液体 LiO 的比质量吸收容量。在含 LiO 的 Li-Na-K 熔融碳酸盐中,CO 主要被碱性氧化物离子(O)吸收。CO 和 CO 之间的化学相互作用有助于通过形成多个碳酸盐离子来吸收 CO。这些吸收离子的传质被发现是控制静态吸收速率的主要因素。较高的温度降低了 CO 吸收的热力学趋势,但升高温度时较低的粘度有利于吸收动力学。与常用的 CaO 吸收剂相比,LiO 在熔融碳酸盐中的溶解度要大得多。含 LiO 的熔融碳酸盐可能是一种很有前途的工业碳捕获和电化学转化过程的介质。