Experimental and theoretical study of the adsorption of mixed low carbon alcohols and acids from Fischer Tropsch synthesis wastewater by activated carbon

Experimental and theoretical study of the adsorption of mixed low carbon alcohols and acids from Fischer Tropsch synthesis wastewater by activated carbon
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活性炭吸附费托合成废水中混合低碳醇酸的实验与理论研究

DOI:
10.1016/j.fuel.2022.126928
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发表时间:
2022-12
期刊:
影响因子:
7.4
通讯作者:
Botao Teng
Botao Teng
中科院分区:
工程技术1区
文献类型:
--
作者:
Yingying Zhang;Baojuan Dou;Xiao Liu;Honglei Fan;Chunyu Geng;Xingchen Liu;Jie Chang;Qinglan Hao;Xin Hu;Yong Yang;Yongwang Li;Botao Teng

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以煤间接液化(FTS)为代表的化工生产过程中会产生大量的含醇含酸废水,因此,采用绿色方法对含醇含酸废水中的低碳醇类和酸类进行高效净化和回收利用具有重要意义。活性炭吸附-脱附法是一种具有工业应用前景的低碳醇和酸类废水处理方法。活性炭对低碳醇和酸的吸附能力与其孔结构和表面性质密切相关。然而,由于炭材料具有不同的孔径、分布和体积,以及表面积和疏水性的复杂性质,这很少被研究。本文选用4种疏水性相近、孔结构和表面结构不同的活性炭材料(AC 1-AC 4),研究了它们对C1-5醇类、C2-4酸类和FTS模拟废水的吸附能力之间的相关性。采用间歇法研究了AC 1 - 104对低碳醇和酸以及FTS模拟废水的吸附能力;采用密度泛函理论(DFT)计算了不同孔径碳纳米管对低碳醇和酸的吸附能。实验和理论计算结果均表明,超微孔对甲醇、乙醇和乙酸的吸附能力有很强的依赖性(<0.9 nm),而戊醇的吸附量主要取决于其相对高的分子量和低的极性;而对C3-C4醇和酸的吸附量与微孔体积和比表面积有很好的相关性。此外,酸的吸附量还与表面COOH物种的含量有关。AC 2因其丰富的超分子量和高的比表面积,对FTS模拟废水中混合低碳醇和酸的吸附容量最高(196.2mg/g)。该研究为开发对低碳醇和酸具有高吸附能力的吸附剂提供了理论和实验依据,为FTS废水的进一步净化和有价值化学品的回收利用提供了理论和实验依据。
To purify and recycle the low-carbon alcohols and acids in wastewater by a green method with high efficiency is of great significance in chemical engineering process, such as indirect coal liquefaction (Fischer Tropsch Synthesis, FTS), which produces a large amount of alcohol and acid-containing wastewater. Adsorption-desorption of low-carbon alcohols and acids in wastewater by activated carbon is a promising method for industrial application. The adsorption capacity of low-carbon alcohols and acids in activated carbons is closely related with their pore and surface properties. However, this was seldom studied due to the complex properties of carbon materials with different pore size, distribution and volume, as well as surface area and hydrophobicity. In this work, four commercial activated carbon materials (AC1 ∼ 4) with similar hydrophobicity and different pore and surface structure were chosen to explore the possible correlation of the adsorption capacity of C1-5 alcohols, C2-4 acids and FTS modeling wastewater. The batch method was used to investigate the adsorption capacity of AC1 ∼ 4 on low-carbon alcohols and acids as well as FTS modeling wastewater; while density functional theory (DFT) calculation was performed to investigate the adsorption energies of low-carbon alcohols and acids in carbon nanotubes with different pore sizes. Both the experimental and theoretical results indicate that the adsorption capacities of methanol, ethanol and acetic acid are strongly dependent on the ultra-micropores (<0.9 nm) due to their small molecular weight; and the adsorption capacity of pentanol is mainly determined by the surface areas due to its relatively high molecular weight and low polarity; while the adsorption capacities of C3-C4 alcohols and acids are well correlated with the microporous volume and surface area. In addition, and the adsorption capacities of acids were also related with the content of surface COOH species. AC2 has the highest adsorption capacity of mixed low-carbon alcohols and acids (196.2 mg/g) in FTS modeling wastewater due to its abundant ultra-micropore and high specific surface area. This work sheds light into the development of adsorbents with high adsorption capacity of low-carbon alcohols and acids, and provides solid experimental and theoretical support in the further purification of FTS wastewater and recovery of valuable chemicals.
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