Shen Junjie, Beale Kai, Amura Ida, Emanuelsson Emma A C
Centre for Advanced Separations Engineering, University of Bath, Bath, United Kingdom.
Department of Chemical Engineering, University of Bath, Bath, United Kingdom.
Front Chem. 2020 May 5;8:375. doi: 10.3389/fchem.2020.00375. eCollection 2020.
Organic solvent nanofiltration (OSN) has been widely applied to separate and recycle homogeneous catalysts, but the influence of ligand and solvent selection on the performance of OSN is not fully understood. Here we prepared four palladium (Pd) catalysts by combining palladium acetate with four ligands of different molecular weights. Morphological and functional properties of the Pd catalysts were characterized by TEM, FTIR, and NMR. OSN experiments were conducted in a lab-scale dead-end filtration rig. Two commercial OSN membranes, PuraMem S600 (PS600) and DuraMem 500 (D500), were used to separate the Pd catalysts from different organic solvents (toluene, isopropanol, butanol/water, and methanol) that are specified to be compatible with, respectively. For both membranes, the pure solvent permeance was positively related to the degree of membrane swelling induced by the solvent. The solvent permeance decreased significantly after the addition of a solute, as a result of membrane fouling and concentration polarization. For the PS600 membrane, the Pd rejection in any solvent was closely correlated to the molecular weight of the ligand, which agrees with the pore-flow model. For the D500 membrane, on the other hand, there was no conclusive link between the Pd rejection and the type of ligand. The one-way analysis of variance (ANOVA) confirmed that the separation processes in PS600 and D500 membranes were controlled by different transport models. The findings shed light on the selection of ligand and solvent in OSN in order to enhance the separation of homogeneous catalysts.
有机溶剂纳滤(OSN)已被广泛应用于分离和回收均相催化剂,但配体和溶剂的选择对OSN性能的影响尚未完全了解。在此,我们通过将醋酸钯与四种不同分子量的配体相结合,制备了四种钯(Pd)催化剂。通过透射电子显微镜(TEM)、傅里叶变换红外光谱(FTIR)和核磁共振(NMR)对钯催化剂的形态和功能特性进行了表征。在实验室规模的死端过滤装置中进行了OSN实验。使用两种商用OSN膜,即PuraMem S600(PS600)和DuraMem 500(D500),分别从指定与之相容的不同有机溶剂(甲苯、异丙醇、丁醇/水和甲醇)中分离钯催化剂。对于这两种膜,纯溶剂渗透率与溶剂引起的膜溶胀程度呈正相关。添加溶质后,由于膜污染和浓差极化,溶剂渗透率显著降低。对于PS600膜,在任何溶剂中钯的截留率与配体的分子量密切相关,这与孔流模型一致。另一方面,对于D500膜,钯的截留率与配体类型之间没有确凿的联系。单因素方差分析(ANOVA)证实,PS600和D500膜中的分离过程受不同的传输模型控制。这些发现为OSN中配体和溶剂的选择提供了启示,以提高均相催化剂的分离效果。