The catalytic effect of calcium and potassium on CO2 gasification of Shengli lignite: the role of carboxyl

The catalytic effect of calcium and potassium on CO2 gasification of Shengli lignite: the role of carboxyl
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钙、钾对胜利褐煤CO 2 气化的催化作用:羧基的作用

DOI:
10.1098/rsos.180717
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发表时间:
2018-09-01
影响因子:
3.5
通讯作者:
Liu, Quansheng
Liu, Quansheng
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Ban, Yanpeng;Wang, Yan;Liu, Quansheng

文献摘要

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以胜利褐煤为原料,研究了K+和Ca 2+催化CO2气化反应。结果表明,钙能显著降低SL的气化反应温度,且钙催化的酸处理SL的气化反应速率显著高于钾催化的酸处理SL。动力学分析表明,钙催化反应的活化能远低于钾催化反应的活化能,这是钙催化活性较高的原因。傅里叶变换红外光谱分析表明,与酸处理的SL相比,K+/Ca 2+的加入使SL中的C=O键明显减弱,并出现了新的羧酸根吸收峰。X-射线光电子能谱(XPS)结果表明,金属离子的加入降低了C=O的数量,形成了金属-羧酸配合物。拉曼表征结果表明,煤样的ID 1/IG值增大,表明煤样的结构缺陷增多,表明煤样的反应活性与无定形碳结构密切相关。Ca ~(2+)与褐煤中羧基结构的相互作用既有离子力作用,也有多羧基配位作用,而K ~+主要通过离子力作用。
The CO2 gasification of Chinese Shengli lignite (SL) catalysed by K+ and Ca2+ was studied. The results showed that calcium could greatly decrease the gasification reaction temperature of SL, and the gasification reaction rates of acid-treated SL catalysed by calcium were significantly higher than that catalysed by potassium. Kinetic analysis showed that the activation energy of the reaction catalysed by calcium was much lower than that catalysed by potassium, which was the reason for the higher catalytic activity of calcium. Fourier transform infrared characterization showed that, compared with acid-treated SL, the addition of K+/Ca2+ resulted in the significant weakening of C=O bond, and new peaks attributed to carboxylate species appeared. X-ray photoelectron spectroscopy results indicated that the numbers of C=O decreased after the metal ions were added, indicating the formation of metal–carboxylate complexes. Raman characterization showed that the ID1/IG values increased, suggesting more structural defects, which indicated that the reactivity of coal samples had a close relation with amorphous carbon structures. Ca2+ could interact with the carboxyl structure in lignite by both ionic forces and polycarboxylic coordination, while K+ interacted with carboxyl structure mainly via ionic forces.