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Membranes 2020, 10, 221 42 of 72 membranes) process for the purification of green tea flavonoids [229], the separation of bioactive peptides [230] and by optimizing the performance of UFMs [231], Bazinet et al. [232] patented the technology. An EDUF cell consists in the stacking of IEMS and UFMs as represented in Figure 22. In this example, positively charged macromolecules selectively migrate from the feed compartment toward the recovery compartment. However, by using an inverted configuration with switched feed and recovery compartments, negative macromolecules could be instead recovered. An improved configuration was developed based on two recovery compartments surrounding the feed compartment [233]. This way, both positive and negative macromolecules could be retrieved. This configuration has been used to selectively separate positive and negative peptides contained in hydrolysates derived from vegetal [234] and animal [235,236] by-products. A limitation of the technique is water transfer. Osmosis phenomena is susceptible to occur due to the difference in concentration between the feed and product compartments, water can then be transferred through the membrane [237]. Although limited in ED, it can be expected in larger proportion in EDUF due to the higher permeability of UFMs compared to IEMs. However, the studies of such phenomenon would need to be supplemented. Recent EDUF advances include the stacking of UFMs with different MWCOs in order to improve size-selectivity as well as the in-situ enzymatic hydrolysis. Hence, the recovery of 4 fractions with two cationic compartments and two anionic compartments was investigated [238,239]. Furthermore, triple selectivity was obtained by stacking three UFMs of decreasing MWCOs [240]. Cationic and anionic configurations were tested. The evaluation of the different fractions in terms of glucose uptake led to the identification of 11 peptides with antidiabetic potential. Interestingly, the lowest-MWCO cationic compartment contained inhibitor peptides and amino acids, while the bioactive peptides were concentrated in the highest-MWCO cationic compartment. To avoid the pre-hydrolysis of the protein before EDUF treatment, Doyen et al. [241] and more recently Suwal et al. [242] tested the simultaneous enzymatic hydrolysis and fractionation of generated bioactive peptide. They observed that the peptide sequence ALPMHIR, identified as lactokinin and known to exert an important antihypertensive effect, was recovered with an estimated 66% migration rate [241] and that the peptide migration rate was found to be affected by the mode of enzymatic hydrolysis and separation [242]. Current research is exploring other ways to optimize hydrolysis before EDUF, e.g., by using high hydrostatic pressure [243]. Recently, Wang et al. [244] synthesized a polyvinylalcohol (PVA) membrane aiming at a 150-kDa MWCO for use as a filtration membrane in an EDUF stack. They experimented on artificial milk in order to selectively recover glycoproteins (lactoferrin and immunoglobulins) and observed promising concentration in the retentate compartment compared to other dairy proteins tested. An alternative EDUF configuration was explored by Tamersit et al. [245] for the desalination of tannery wastewaters. By protecting the AEM with an UFM in the electrodialytic cell, they managed to totally prevent peptide and protein fouling. Pulsed electric fields and polarity reversal were also studied in EDUF as a way to prevent fouling [105]. Both modes reduced significantly fouling, especially on AEMs, while PEF (2 s pulse/0.5 s pause) provided an increased selectivity for arginine and lysine-based peptides compared to direct current mode. In 2020, predictive models were developed for determination of peptide fouling [246] and peptide migration/selectivity [247] based on the physicochemical characteristics of the filtration membranes (conductivity, contact angle, % of hydrophilic pores, porosity, zeta-potential, Arithmetic mean of roughness Ra and Maximum height Rz), their pore size (from 5 kDa to 300 kDa) and their material (PES, PAN, PVDF and PVC-silica). The mechanisms involved in the fouling of peptide and their migration were also deeply studied as a function of these characteristics [246,247]. The recent breakthrough regarding PEF applied to ED technologies should promote their future investigation in EDUF for low-cost and efficient processes. In the same vein, although a preliminary study was carried out regarding overlimiting conditions in EDUF [248], additional exploration of electroconvection in EDUF would benefit to the field. The scale-up of this technology at a pre-industrial scale, in collaboration with an equipment manufacturer, is currently underway in our team for bioactive peptide separation.PDF Image | Electrodialytic Processes
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