Unlocking high-performance HCl adsorption at elevated temperatures: the synthesis and characterization of robust Ca–Mg–Al mixed oxides

Environmental Science and Pollution Research(2024)

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摘要
The presence of HCl and SO2 gas imposes limitations on syngas utilization obtained from household waste in a wide range of applications. The hydrotalcite-like compounds (HTLs) have been proved that could remove HCl efficiency. However, the research on impact of synthesis conditions of HTLs and SO2 on HCl removal was limited. In this study, a range of Ca–Mg–Al mixed oxide sorbents was synthesized by calcining HTLs, with variations in crystallization temperature, solution pH, and the Ca/Mg molar ratio. These sorbents were examined for their effectiveness in removing HCl at medium–high temperatures under diverse conditions. The adsorption performance of selected sorbents for the removal of HCl, SO2, and HCl-SO2 mixed gas at temperature of 350 °C, 450 °C, and 550 °C, respectively, was evaluated using thermogravimetric analysis (TGA). It was observed that the HTL synthesis parameters significantly influenced the HCl adsorption capacity of Ca–Mg–Al mixed oxides. Notably, HTLs synthesized at 60 °C, a solution pH of 10–11, and a Ca/Mg ratio of 4 exhibited superior crystallinity and optimal adsorption characteristics. For individual HCl and SO2 removal, temperature had a minor effect on HCl adsorption but significantly impacted SO2 adsorption rates. At temperatures above 550 °C, SO2 removal efficiency substantially decreased. When exposed to a mixed gas, the Ca–Mg–Al mixed oxides could efficiently remove both HCl and SO2 at temperatures below 550 °C, with HCl dominating the adsorption process at higher temperatures. This dual-action capability is attributed to several mechanisms through which HTL sorbents interacted with HCl, including pore filling, ion exchange, and cation exchange. Initially, HCl absorbed onto specific sites created by water and CO2 removal due to the surface’s polarity. Subsequently, HCl reacted with CaCO3 and CaO formed during HTL decomposition.
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关键词
Synthesis,Hydrotalcite-like compounds,HCl,SO2,Adsorption
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