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氧化石墨烯膜从溶剂-水混合物中对木质素模型化合物进行选择性分子分离

Selective molecular separation of lignin model compounds by reduced graphene oxide membranes from solvent-water mixture.

作者信息

Aher Ashish, Sarma Rupam, Crocker Mark, Bhattacharyya Dibakar

机构信息

Dept. Chemical and Materials Engineering, University of Kentucky, Lexington, KY 40506, USA.

Center for Applied Energy Research, Lexington, KY 40511, USA.

出版信息

Sep Purif Technol. 2020 Jan 2;230. doi: 10.1016/j.seppur.2019.115865. Epub 2019 Jul 27.

Abstract

Selective separation of lignin depolymerization products is key to fractionating and isolating high-value aromatic compounds from the depolymerization process. The primary aim of this study was to synthesis graphene oxide (GO) membranes for selective separations of lignin oligomeric units from polar organic solvent-water media. GO membranes were synthesized on a polymeric substrate by a shear assisted casting of aqueous GO dispersion using a wire-wound rod. Deposited GO was then reduced to different extents by controlled thermal incubation, and the impact on membrane performance was investigated. The extent of reduction of GO was established by extensive characterization with FTIR, XPS, Raman Spectroscopy, XRD, and contact angle measurements. Impressive performance with the rejection of over 70% for the model compound trimer BMP (2,6-bis[(2-hydroxy-5-methyl phenyl) methyl]-4-methylphenol) was achieved compared to only 20% rejection for the dimer GGE (guaiacylglycerol-β-guaiacylether) with isopropanol-water (90-10% by volume) as a solvent. This corresponds to an encouraging selective separation with selective permeation of dimer (GGE) 3.5 times higher compared to trimer (BMP). rGO membranes exhibited a stable performance over 84 h of operation at a shear rate of 1.1 Pa in a cross-flow mode of operation. Selective separation of GO can be effectively modulated by controlling the O/C ratio by the extent of reduction of GO; indeed, the retention of trimeric compounds increased with increasing GO reduction. The remarkable performance of GO membranes could enable energy-efficient fractionation of lignin oligomeric compounds from polar organic solvents.

摘要

木质素解聚产物的选择性分离是从解聚过程中分馏和分离高价值芳香族化合物的关键。本研究的主要目的是合成氧化石墨烯(GO)膜,用于从极性有机溶剂 - 水介质中选择性分离木质素低聚单元。通过使用绕线棒对GO水分散体进行剪切辅助浇铸,在聚合物基底上合成GO膜。然后通过控制热孵育将沉积的GO在不同程度上还原,并研究其对膜性能的影响。通过傅里叶变换红外光谱(FTIR)、X射线光电子能谱(XPS)、拉曼光谱、X射线衍射(XRD)和接触角测量等广泛表征确定了GO的还原程度。与以异丙醇 - 水(体积比90 - 10%)为溶剂时二聚体GGE(愈创木基甘油 - β - 愈创木基醚)仅20%的截留率相比,该膜对模型化合物三聚体BMP(2,6 - 双[(2 - 羟基 - 5 - 甲基苯基)甲基] - 4 - 甲基苯酚)的截留率超过70%,表现出令人印象深刻的性能。这对应于令人鼓舞的选择性分离,二聚体(GGE)的选择性渗透率比三聚体(BMP)高3.5倍。在错流操作模式下,rGO膜在1.1 Pa的剪切速率下运行84小时表现出稳定的性能。通过控制GO的还原程度来调节O/C比,可以有效地调控GO的选择性分离;实际上,三聚体化合物的保留率随着GO还原程度的增加而增加。GO膜的卓越性能能够实现从极性有机溶剂中对木质素低聚化合物进行节能分馏。

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