Gout flare-up, commonly resulting from monosodium urate monohydrate (MSUM) crystallization, has led to painful inflammatory arthritis among hundreds of millions of people. Herein, a kind of hydrogel nanoparticles (HNPs) with specific properties was developed, aimed at providing a promising pathway for MSUM crystallization control. The experimental and molecular dynamics simulation results synchronously indicate that the fabricated HNPs achieve efficient inhibition of MSUM crystallization governed by the mechanism of "host-guest interaction" even under very low-dose administration. HNPs as the host dispersed in the hyperuricemic model effectively lift the relative heterogeneous nucleation barrier of the MSUM crystal and hinder solute aggregation with strong electronegativity and hydrophobicity. The initial appearance of MSUM crystals was then delayed from 94 to 334 h. HNPs as the guest on the surface of the formed crystal can decelerate the growth rate by anchoring ions and occupying the active sites on the surface, and the terminal yield of the MSUM crystal declined to less than 1% of the control group. The good biocompatibility of HNPs (cell viability > 94%) renders it possible for future clinical applications. This study can guide the rational design of inhibitory nanomaterials and the development of their application in the control of relevant pathological crystallization.
Herein, membrane-assisted reactive crystallization (MARC) with effective interfacial flow regimes was proposed to achieve the effective mass transfer control during reactive crystallization. Three tube-shell side solution systems (EtOH-H2O, Butanol-H2O and H2O-H2O) were chosen to form different flow regimes on the membrane surface, including the microscale liquid layer and the uniform droplets. The fundamen-tal mechanisms of 'rising and falling tide' phenomenon, and flexible layer thickness control were uncov-ered. A force analysis model was established to illustrate the transition behavior of the droplet and liquid layer on the membrane surface. Molecular simulations additionally demonstrated that MARC imple-mented various ion diffusion conditions in different solution systems. Compared to the conventional reactive crystallization, MARC with multiple flow regimes can achieve effective control of CaCO3 crystal size ranging from 700 nm to 3 lm and obtain uniform size distribution (coefficient of variation less than 15.1 %), which shed light on the advanced material manufacture with reactive crystallization process.
Herein, a facile bionic research platform with fabricated hydrogel composite membrane (HCM) is constructed to uncover the effects of the main components of coffee's metabolites on MSUM crystallization. Tailored and biosafety polyethylene glycol diacrylate/N-isopropyl acrylamide (PEGDA/NIPAM) HCM allows the proper mass transfer of coffee's metabolites and can well simulate the process of coffee's metabolites acting in the joint system. With the validations of this platform, it is shown that chlorogenic acid (CGA) can hinder the MSUM crystals formation from 45 h (control group) to 122 h (2 mM CGA), which is the most likely reason that reduces the risk of gout after long-term coffee consumption. Molecular dynamics simulation further indicates that the high interaction energy (Eint) between CGA and MSUM crystal surface and the high electronegativity of CGA both contribute to the restraint of MSUM crystal formation. In conclusion, the fabricated HCM, as the core functional materials of the research platform, presents the understanding of the interaction between coffee consumption and gout control.
Antisolvent engineering is routinely used to modulate the crystallization of perovskite films as they can offer an additional driving force for nucleation. Actually, the intervention of antisolvent into nucleation is thought to involve some relatively fast and complex processes, which, however, are not fully understood so far. Here, the diffusion of the organic amine cation FA+ (one dominated precursor) and its distribution in a spin-coating process in different antisolvents is simulated by the computational fluid dynamics (CFD) model. It is suggested that a moderate diffusion rate (like that in the case of toluene as an antisolvent) not only enables to form a very uniform distribution of FA+ ions on the substrate, beneficial to the uniform nucleation of the intermediate phase, but also can balance the nucleation and growth rates of the intermediate phase, thereby suppressing undesired heterogeneous nucleation and growth. Results show that the perovskite film fabricated using toluene as an antisolvent has a high quality, based on which higher power conversion efficiencies of up to 24.32% are achieved for perovskite solar cells.
Nanofiltration (NF) is a promising technique to achieve sustainable and efficient separation of antibiotics with high industrial value. In this work, carboxymethyl-S-cyclodextrin (CM-S-CD) modified nanofiltration membrane was fabricated through interfacial polymerization (IP) for high concentration cephalexin solution separation, which is a classic antibiotic pharmaceutical wastewater. In principle, CM-S-CD can slow down the diffusion of amine monomers via electrostatic attraction, steric effect, hydrogen bonding and adsorption of the piperazine (PIP) monomer onto the hydrophilic surface, which renders amine monomer the high local concentration. The fabricated NF membranes possessed a larger proportion of dense primary layer on the surface. In addition, the accumulation of CM-S-CD between the substrate membrane and polyamide (PA) layer played the role as a barrier with specific cavity structure and bulk carboxylate to enhance the rejection of cephalexin. The cavity structure and stacking gap of CM-beta-CD simultaneously rendered the membrane interlayer highly permeable. The optimal CM-S-CD modified membrane exhibited high rejection of cephalexin (94.7%) and water permeability of 122.4 L m-2 h-1 MPa- 1 when the concentration of cephalexin was 3473.9 ppm (10 mmol/L). This work furnished an available way to prepare a novel nanofiltration membrane with efficient separation performance for relevant pharmaceutical production wastewater.
Gout is the most common of inflammatory arthropathy caused by the crystallization and accumulation of monosodium urate monohydrate (MSUM) in joints. Herein, fabricated hydrogel composited membrane (HCM) is developed to simulate the mass transfer in joints. A facile and versatile HCM based dynamic platform is established to investigate the “triggers” mechanism of gout under alcohol and its metabolites (acetaldehyde (AH) and acetic acid (HAc) intake condition. The distinct role of EtOH on enhanced gout onset was demonstrated, which attributes to the low interaction energy (Eint) between EtOH and the main crystal surface. While, HAc and carboxyl groups exhibit potentially restrain the MSUM crystallization. This conclusion is furtherly confirmed by the different restraint performance of two kinds of fabricated HCM. PEGDA/AA (polyethylene glycol diacrylate/acrylic acid) with abundant carboxyl groups can delay the appearance time of MSUM crystals from 20 h to 82 h and reduce the crystal yield to 7.5% of the one via PEGDA/NIPAM (N-isopropylacrylamide). The excellent electronegativity of PEGDA/AA renders the adsorption of sodium ion on the HCM interface, which furtherly increases the nucleation energy barrier of MSUM crystal. The functional HCM based platform can guide the relevant biomedical research and rational drug design for gout prevention.