High-Performance Flexible Hybrid Silica Membranes with an Ultrasonic Atomization-Assisted Spray-Coated Active Layer on Polymer for Isopropanol Dehydration.

Organic-inorganic hybrid silica materials, incorporating an organic group bridging two silicon atoms, have demonstrated great potential in creating membranes with excellent permselectivity. Yet, the large-scale production of polymer-supported flexible hybrid silica membranes has remained a significant challenge. In this study, we present an easy and scalable approach for fabricating these membranes. By employing a sol-gel ultrasonic spray process with a single-pass method, we deposited a thin and uniform hybrid active layer onto a porous polymer substrate. We first optimized the deposition conditions, including substrate temperature, the binary solvent ratio of the silica sol, and various ultrasonic spray parameters. The resulting flexible hybrid silica membranes exhibited exceptional dehydration performance for isopropanol (IPA)/water solutions (IPA: 90 wt%) in the pervaporation process, achieving a water flux of 0.6 kg/(m2 h) and a separation factor of around 1300. This work demonstrates that the single-pass ultrasonic spray method is an effective strategy for the large-scale production of polymer-supported flexible hybrid silica membranes.

2,2'-Biphenol-based Ultrathin Microporous Nanofilms for Highly Efficient Molecular Sieving Separation.

Organic solvent nanofiltration (OSN) is an emerging membrane separation technology, which urgently requires robust, easily processed, OSN membranes possessing high permeance and small solutes-selectivity to facilitate enhanced industrial uptake. Herein, we describe the use of two 2,2'-biphenol (BIPOL) derivatives to fabricate hyper-crosslinked, microporous polymer nanofilms through IP. Ultra-thin, defect-free polyesteramide/polyester nanofilms (≈5 nm) could be obtained readily due to the relatively large molecular size and ionized nature of the BIPOL monomers retarding the rate of the IP. The enhanced microporosity arises from the hyper-crosslinked network structure and monomer rigidity. Specifically, the amino-BIPOL/PAN membrane exhibits extraordinary permselectivity performances with molecular weight cut-off as low as 233 Da and MeOH permeance of ≈13 LMH/bar. Precise separation of small dye mixtures with similar M.W. based on both their charge and molecular size are achieved.

Thin-Film Composite Membranes with a Carbon Nanotube Interlayer for Organic Solvent Nanofiltration.

Compared to the traditional chemical-crosslinking-based polymer, the porous polytetrafluoroethylene (PTFE) substrate is considered to be an excellent support for the fabrication of thin-film composite (TFC) organic solvent nanofiltration (OSN) membranes. However, the low surface energy and chemical inertness of PTFE membranes presented major challenges for fabricating a polyamide active layer on its surface via interfacial polymerization (IP). In this study, a triple-layered TFC OSN membrane was fabricated via IP, which consisted of a PA top layer on a carbon nanotube (CNT) interlayer covering the macroporous PTFE substrate. The defect-free formation and cross-linking degree of the PA layer can be improved by controlling the CNT deposition amount to achieve a good OSN performance. This new TFC OSN membrane exhibited a high dye rejection (the rejection of Bright blue B > 97%) and a moderate and stable methanol permeated flux of approximately 8.0 L m−2 h−1 bar−1. Moreover, this TFC OSN membrane also exhibited an excellent solvent resistance to various organic solvents and long-term stability during a continuous OSN process.

New Insights into the Role of an Interlayer for the Fabrication of Highly Selective and Permeable Thin-Film Composite Nanofiltration Membrane.

A triple-layered TFC nanofiltration (NF) membrane consisting of a polyamide (PA) top layer covered on a poly(ether sulfone) microfiltration membrane with a carbon nanotube (CNT) interlayer was fabricated via interfacial polymerization. The structure and properties of the PA active layer could be finely tailored by tuning the interfacial properties and pore structure of the CNT interlayer, including its surface pore size and thickness, thus improving its NF performance. This TFC NF membrane exhibited a high divalent salt rejection (the rejection of Na2SO4 and MgSO4 solution >98.3%) and dye rejection (the rejection of methyl violet (MV) >99.5%) with a high pure water flux of around 21 L m-2 h-1 bar-1. Excitingly, this membrane also showed excellent selectivity to both mono/divalent salt ion (the selectivity of Cl-/SO42- is as high as 85.5) and NaCl/dye solution (the selectivity of NaCl/MV is more than 123.5), which are much higher than most of other commercial and reported NF membranes. Moreover, this membrane also showed a good separation performance and long-term stability during a continuous NF process for a salt/dye mixture solution. This triple-layered TFC NF membrane showed a great promise for applications in both wastewater treatment and dyes recycling.

Facile and Scalable Flow-Induced Deposition of Organosilica on Porous Polymer Supports for Reverse Osmosis Desalination.

The fabrication of a continuous and uniform organosilica membrane on a porous polymer substrate was achieved via a facile and technologically scalable flow-induced deposition (FD) approach. The uniformity of the thickness of an organosilica separation layer on a polymer surface with a large area was improved significantly via this two-step FD approach. Meanwhile, the optimal concentration of the organosilica used in membrane preparation was also investigated. This polymer-supported organosilica layered-hybrid membrane showed a high level of NaCl rejection (97.5-99%) in the reverse osmosis desalination of a 2000 ppm NaCl solution at an operating pressure of 3 MPa. This membrane also exhibited good stability and flexibility when rolled into a curvature radius of 11 mm.

Yeast Microcapsule-Mediated Targeted Delivery of Diverse Nanoparticles for Imaging and Therapy via the Oral Route.

Targeting of nanoparticles to distant diseased sites after oral delivery remains highly challenging due to the existence of many biological barriers in the gastrointestinal tract. Here we report targeted oral delivery of diverse nanoparticles in multiple disease models, via a "Trojan horse" strategy based on a bioinspired yeast capsule (YC). Diverse charged nanoprobes including quantum dots (QDs), iron oxide nanoparticles (IONPs), and assembled organic fluorescent nanoparticles can be effectively loaded into YC through electrostatic force-driven spontaneous deposition, resulting in different diagnostic YC assemblies. Also, different positive nanotherapies containing an anti-inflammatory drug indomethacin (IND) or an antitumor drug paclitaxel (PTX) are efficiently packaged into YC. YCs containing either nanoprobes or nanotherapies may be rapidly endocytosed by macrophages and maintained in cells for a relatively long period of time. Post oral administration, nanoparticles packaged in YC are first transcytosed by M cells and sequentially endocytosed by macrophages, then transported to neighboring lymphoid tissues, and finally delivered to remote diseased sites of inflammation or tumor in mice or rats, all through the natural route of macrophage activation, recruitment, and deployment. For the examined acute inflammation model, the targeting efficiency of YC-delivered QDs or IONPs is even higher than that of control nanoprobes administered at the same dose via intravenous injection. Assembled IND or PTX nanotherapies orally delivered via YCs exhibit remarkably potentiated efficacies as compared to nanotherapies alone in animal models of inflammation and tumor, which is consistent with the targeting effect and enhanced accumulation of drug molecules at diseased sites. Consequently, through the intricate transportation route, nanoprobes or nanotherapies enveloped in YC can be preferentially delivered to desired targets, affording remarkably improved efficacies for the treatment of multiple diseases associated with inflammation.

Tailoring the Separation Behavior of Polymer-Supported Organosilica Layered-Hybrid Membranes via Facile Post-Treatment Using HCl and HN3 Vapors.

A promising layered-hybrid membrane consisting of a microporous organosilica active layer deposited onto a porous polymer support was prepared via a facile sol-gel spin-coating process. Subsequently, the pore sizes and structures of the organosilica top layers on the membrane surface were tuned at mild temperature combined with vapor treatment from either hydrochloric acid (HVT) or ammonia (AVT), thereby tailoring the desalination performance of the membranes during reverse osmosis (RO) processing. The effects of HVT and AVT on the pore size, structure, and morphology of organosilica layers and on the separation performances of membranes were investigated in detail. We confirmed that both HVT and AVT processes accelerated the condensation of silanol (Si-OH) in the organosilica layer, which led to dense silica networks. The layered-hybrid membranes after HVT showed an improved salt rejection and reduced water flux, while membranes after AVT exhibited a decrease in both salt rejection and water permeability. We found that HVT gave rise to smoother and denser organosilica layers, while AVT produced large voids and formed pinholes due to Ostwald ripening. These conclusions were supported by a comparative analysis of the results obtained via FTIR, TG-MS, SPM, and RO desalination.

Characterization of alcohol dehydrogenase from permeabilized brewer's yeast cells immobilized on the derived attapulgite nanofibers.

Alcohol dehydrogenase (ADH) from permeabilized brewer's yeast was immobilized on derived attapulgite nanofibers via glutaraldehyde covalent binding. The effect of immobilization on ADH activity, optimum temperature and pH, thermal, pH and operational stability, reusability of immobilized ADH, and bioreduction of ethyl 3-oxobutyrate (EOB) to ethyl(S)-3-hydroxybutyrate ((S)-EHB) by the immobilized ADH were investigated. The results show the immobilized ADH retained higher activity over wider ranges of pH and temperature than those of the free. The optimum temperature and pH were 7.5 and 35 degrees C, respectively, and 58% of the original activity was retented after incubation at 35 degrees C for 32 h. More importantly, in bioreduction of EOB mediated by immobilized ADH, the conversion of substrate and enantiomeric excess (ee) of product reached 88% and 99.2%, respectively, within 2 h and retained about 42% of the initial activity after eight cycles.

Effects of industrial storage on the bioreduction capacity of brewer's yeast.

The effects of industrial storage on the changes of the cell viability and the activities of intracellular alcohol dehydrogenase (ADH) and glucose-6-phosphate dehydrogenase (G6PDH) in brewer's yeast, and the corresponding capacity for the bioconversion of ethyl-3-oxobutanoate (EOB) to ethyl (S)-3-hydroxybutanoate ((S)-EHB), were investigated. The viability of fresh brewer's yeast cells stored in industrial circulating cooling water at 1-2 degrees C showed 4 and 15% drop after the storage of 7 and 15 days, respectively, after which cells died rapidly. The pretreatment of the stored brewer's yeast cells by washing and screening significantly enhanced cell viability during industrial storage. The intracellular levels of ADH and G6PDH after permeabilization of these stored cells with cetyltrimetylammonium bromide (CTAB) were much higher, which showed only slight decrease within 2 weeks during the industrial storage. When the stored cells after the permeabilization treatment was used as the biocatalyst at 90-120 g/L, EOB was converted almost completely into enantiopure (S)-EHB with an enantiomeric excess (ee) more than 99% and a yield of over 96%, by fed-batch bioconversion of 560 mM EOB within 6 h.