Browsing by Author "Liu, Jianzhao"

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    Bulk and interfacial interactions between hydroxypropyl-cellulose and bile salts: Impact on the digestion of emulsified lipids
    Zornjak, Jennifer; Liu, Jianzhao; Esker, Alan R.; Lin, Tiantian; Fernández-Fraguas, Cristina (2020-09)
    Hydroxypropyl-cellulose (HPC) is a surface-active, non-digestible polysaccharide, commonly used in food emulsions as thickener and/or emulsifier. Due to these dual characteristics, HPC is a potential ingredient to modulate lipid digestion. Since bile salts (BS) are key players during lipid digestion, the aim of this work was to investigate the impact that interactions of HPC with BS has on the digestion of emulsified lipids. We studied the effect of two BS species differing in bile-acid moiety, sodium-taurocholate (NaTC) and sodium-taurodeoxycholate (NaTDC). A Quartz-Crystal-Microbalance (QCM-D) was used to evaluate HPC-BS interfacial interactions during the sequential and simultaneous adsorption of both components at a hydrophobic surface, while microDifferential-Scanning-Calorimetry was used to examine bulk interactions. In vitro lipid digestion was studied by using a pH-stat method. Results showed that, under fed-state conditions, NaTDC micelles were more effective at displacing a pre-adsorbed HPC layer from the surface than NaTC monomers. Nevertheless, HPC was resistant to complete displacement by both BS. Additionally, HPC was more susceptible to interact with NaTDC in the bulk, compared to NaTC, which made the adsorption more competitive for NaTDC. The reduced amount of free NaTDC in solution could explain the delayed lipolysis shown by HPC-stabilized emulsions when NaTDC was used to simulate duodenal conditions. These findings show that the delay of lipid digestion by HPC is due to the combined effect of HPC-BS interfacial and bulk interactions, with BS-binding in solution mostly contributing to this effect, and the BS molecular and micellar structure playing essential roles on both situations.
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    Regulating the Hidden Solvation-Ion-Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries
    Amine, Rachid; Liu, Jianzhao; Acznik, Ilona; Sheng, Tian; Lota, Katarzyna; Sun, Hui; Sun, Cheng-Jun; Fic, Krzysztof; Zuo, Xiaobing; Ren, Yang; Abd El-Hady, Deia; Alshitari, Wael; Al-Bogami, Abdullah S.; Chen, Zonghai; Amine, Khalil; Xu, Gui-Liang (2020-07)
    Lithium-sulfur batteries are attractive for automobile and grid applications due to their high theoretical energy density and the abundance of sulfur. Despite the significant progress in cathode development, lithium metal degradation and the polysulfide shuttle remain two critical challenges in the practical application of Li-S batteries. Development of advanced electrolytes has become a promising strategy to simultaneously suppress lithium dendrite formation and prevent polysulfide dissolution. Here, a new class of concentrated siloxane-based electrolytes, demonstrating significantly improved performance over the widely investigated ether-based electrolytes are reported in terms of stabilizing the sulfur cathode and Li metal anode as well as minimizing flammability. Through a combination of experimental and computational investigation, it is found that siloxane solvents can effectively regulate a hidden solvation-ion-exchange process in the concentrated electrolytes that results from the interactions between cations/anions (e.g., Li+, TFSI-, and S2-) and solvents. As a result, it could invoke a quasi-solid-solid lithiation and enable reversible Li plating/stripping and robust solid-electrolyte interphase chemistries. The solvation-ion-exchange process in the concentrated electrolytes is a key factor in understanding and designing electrolytes for other high-energy lithium metal batteries.
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    Seed-mediated biomineralizaton toward the high yield production of gold nanoprisms
    Geng, Xi; Roth, Kristina L.; Freyman, Megan C.; Liu, Jianzhao; Grove, Tijana Z. (Royal Society of Chemistry, 2016-07-12)
    Gold nanotriangles (Au NTs) with tunable edge length were synthesized via a green chemical route in the presence of the designed consensus sequence tetratricopeptide repeat (CTPR) protein, halide anions (Br−) and CTPR-stabilized Ag seeds. The well-defined morphologies, tailored plasmonic absorbance from visible-light to the near infrared (NIR) region, colloidal stability and biocompatibility are attributed to the synergistic action of CTPR, halide ions, and CTPR-stabilized Ag seeds.
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    Studies of Macromolecule/Molecule Adsorption and Activity at Interfaces
    Liu, Jianzhao (Virginia Tech, 2020-01-03)
    Interfaces are ubiquitous in our daily life. A good understanding of the interfacial properties between different materials, or a single material in different physical states is of critical importance for us to explore the current world and bring benefits to mankind. In this work, interfacial behavior was investigated with the help of surface analysis techniques, such as quartz crystal microbalance with dissipation monitoring (QCM-D), surface plasmon resonance (SPR) and atomic force microscopy (AFM), in order to gain better understanding on biofuel conversion, gene/drug delivery, and chemical fixation of CO2. Biomimetic chelator-mediated Fenton (CMF) non-enzymatic degradations on cellulose and chitin thin films was studied by liquid-phase QCM-D and AFM. QCM-D is a powerful tool to monitor the kinetics of hydrolysis of regenerated cellulose and chitin model surfaces. Results from QCM-D and AFM showed that the majority of the biomass of the two model surfaces can be hydrolyzed by the CMF system. The initial degradation rates for both model surfaces by the CMF system are faster than that of the corresponding enzyme systems. The CMF system, which is a good non-enzymatic pretreatment agent for cellulose and chitin, may work on a wide variety of polysaccharide systems. Adsorption of cationic cellulose derivatives onto self-assembled monolayer (SAM) surfaces was investigated using liquid-phase SPR. Results from SPR showed that depending upon the cellulose derivative structure, irreversible adsorption ranging from a monolayer to ~1.6 layers of cellulose derivative were formed on the SAM-COOH surface based upon a charge neutralization mechanism. At low salt concentrations, the long-range electrostatic attraction between the cationic cellulose derivatives (6-PyrCA and 6-MeIMCA) and the SAM surfaces facilitates the formation of a 2-dimensional monolayer. While, for TMACE, the energy gained through the hydrophobic interaction between adjacent long polyelectrolyte branches may afford the electrostatic repulsion and chain entropy penalties, resulting in the formation of 3-dimensional adsorbed polyelectrolyte layers. Adsorption of 1,2-epoxybutane gas molecules onto/into VPI-100 metal–organic frameworks (MOFs) was studied by gas-phase QCM-D experiments. Results from QCM-D demonstrated that VPI-100 (Ni) MOFs have higher irreversible adsorption per unit cell (θ) and faster diffusion coefficients (D) than VPI-100 (Cu) MOFs. The presence of bound counter-balancing ions on the metallo-cyclam core was attributed as the cause of the higher θ and faster D through the Ni analogue, which suggests the MOF-epoxide interaction occurs at the metallo-cyclam. This study shed light upon tuning MOF structures for better CO2 sorption and epoxide activation to gain higher catalytic efficiency. Finally, in operando high energy X-ray diffraction (HEXRD) was used to monitor the phase transition of the NaxNi1/3Co1/3Mn1/3O2 cathode material during the sintering process. The first charge/discharge cycle of the NaxNi1/3Co1/3Mn1/3O2 cathode materials in different phases were also studied by in operando HEXRD. It was found that the intergrowth P2/O1/O3 cathode (NCM-Q cathode) can inhibit the irreversible P2–O2 phase transition and simultaneously improve the structural stability of the O3 and O1 phases during cycling. The NCM-Q cathode with triple-phase integration demonstrates highly reversible phase evolution during high voltage cycling, possibly leading to a highly reversible capacity and good cycle stability.