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Yang, Liye; Li, Wenying; Huang, Yanyu; Zhou, Yangliang; Chen, Tianfeng
doi: 10.1002/marc.201570067pmid: N/A
Front Cover: A RGD peptide is covalently conjugated to a fluorescent selenocompound BSeC using polyethylenimine as a linker, which forms a nanosystem in aqueous solution. This rational design effectively enhances the selective cellular uptake of BSeC in human glioma cells, and increases its selectivity between cancer and normal cells. Further details can be found in the article by L. Yang, W. Li, Y. Huang, Y. Zhou, and T. Chen* on page 1559.
Guo, Kai; Guo, Zaihong; Ludlow, James M.; Xie, Tingzheng; Liao, Shengyun; Newkome, George R.; Wesdemiotis, Chrys
doi: 10.1002/marc.201500084pmid: 26248126
Top‐down multidimensional mass spectrometry, interfacing electrospray ionization (ESI) with ion mobility mass spectrometry (IM‐MS), and energy resolved (gradient) tandem mass spectrometry (gMS2) are employed to characterize the stoichiometries, architectures, and intrinsic stabilities of coordinatively bound supramolecular polymers containing terpyridine functionalized ligands. As a soft ionization method, ESI prevents or minimizes unwanted assembly destruction. The IM dimension affords separation of the supramolecular ions by charge and collision cross‐section (a function of size and shape). The mobility separated ions are subsequently identified by their mass‐to‐charge‐ratios and isotope patterns in the orthogonal MS dimension. Finally, the gMS2 dimension reveals bond breaking proclivities and disintegration pathways of the assemblies. The described methodology does not require high sample purity due to the dispersive nature of the IM and MS steps. Its utility is demonstrated with the comprehensive analysis of bisterpyridine‐based metallomacrocycle mixtures and a tristerpyridine based complex with 3‐D nanosphere‐like architecture.
Yang, Xinjia; Tan, Liangxiao; Xia, Lingling; Wood, Colin D.; Tan, Bien
doi: 10.1002/marc.201500235pmid: 26178423
Hierarchical porous polystyrene monoliths (HCP‐PolyHIPE) are obtained by hypercrosslinking poly(styrene‐divinylbenzene) monoliths prepared by polymerization of high internal phase emulsions (PolyHIPEs). The hypercrosslinking is achieved using an approach known as knitting which employs formaldehyde dimethyl acetal (FDA) as an external crosslinker. Scanning electron microscopy (SEM) confirms that the macroporous structure in the original monolith is retained during the knitting process. By increasing the amount of divinylbenzene (DVB) in PolyHIPE, the BET surface area and pore volume of the HCP‐PolyHIPE decrease, while the micropore size increases. BET surface areas of 196–595 m2 g−1 are obtained. The presence of micropores, mesopores, and macropores is confirmed from the pore size distribution. With a hierarchical porous structure, the monoliths reveal comparable gas sorption properties and potential applications in oil spill clean‐up.
Yang, Liye; Li, Wenying; Huang, Yanyu; Zhou, Yangliang; Chen, Tianfeng
doi: 10.1002/marc.201500243pmid: 26205253
A cancer‐targeted conjugate of the selenadiazole derivative BSeC (benzo(1,2,5) selenadiazole‐5‐carboxylic acid) with RGD peptide as targeting molecule and PEI (polyethylenimine) as a linker is rationally designed and synthesized in the present study. The results show that RGD‐PEI‐BSeC forms nanoparticles in aqueous solution with a core–shell nanostructure and high stability under physiological conditions. This rational design effectively enhances the selective cellular uptake and cellular retention of BSeC in human glioma cells, and increases its selectivity between cancer and normal cells. The nanoparticles enter the cells through receptor‐mediated endocytosis via clathrin‐mediated and nystatin‐dependent lipid raft‐mediated pathways. Internalized nanoparticles trigger glioma cell apoptosis by activation of ROS‐mediated p53 phosphorylation. Therefore, this study provides a strategy for the rational design of selenium‐containing cancer‐targeted theranostics.
Xiang, Lu; Zhu, Yunlong; Gu, Shuai; Chen, Dongyang; Fu, Xian; Zhang, Yindong; Yu, Guipeng; Pan, Chunyue; Hu, Yuehua
doi: 10.1002/marc.201500159pmid: 26088466
A hypercrosslinked conjugated microporous polymer (HCMP‐1) with a robustly efficient absorption and highly specific sensitivity to mercury ions (Hg2+) is synthesized in a one‐step Friedel–Crafts alkylation of cost‐effective 2,4,6‐trichloro‐1,3,5‐triazine and dibenzofuran in 1,2‐dichloroethane. HCMP‐1 has a moderate Brunauer–Emmett–Teller specific surface (432 m2 g−1), but it displays a high adsorption affinity (604 mg g−1) and excellent trace efficiency for Hg2+. The π–π* electronic transition among the aromatic heterocyclic rings endows HCMP‐1 a strong fluorescent property and the fluorescence is obviously weakened after Hg2+ uptake, which makes the hypercrosslinked conjugated microporous polymer a promising fluorescent probe for Hg2+ detection, owning a super‐high sensitivity (detection limit 5 × 10−8 mol L−1).
Clarkson, Christopher G.; Lovett, Joseph R.; Madsen, Jeppe; Armes, Steven P.; Geoghegan, Mark
doi: 10.1002/marc.201500208pmid: 26096738
The temperature and pH‐dependent diffusion of poly(glycerol monomethacrylate)‐block‐poly(2‐hydroxypropyl methacrylate) nanoparticles prepared via polymerization‐induced self‐assembly in water is characterized using fluorescence correlation spectroscopy (FCS). Lowering the solution temperature or raising the solution pH induces a worm‐to‐sphere transition and hence an increase in diffusion coefficient by a factor of between four and eight. FCS enables morphological transitions to be monitored at relatively high copolymer concentrations (10% w/w) compared to those required for dynamic light scattering (0.1% w/w). This is important because such transitions are reversible at the former concentration, whereas they are irreversible at the latter. Furthermore, the FCS data suggest that the thermal transition takes place over a very narrow temperature range (less than 2 °C). These results demonstrate the application of FCS to characterize order–order transitions, as opposed to order–disorder transitions.
Ding, Liang; Qiu, Jun; Li, Juan; Wang, Chengshuang; Wang, Lingfang
doi: 10.1002/marc.201500230pmid: 26098645
Novel photoresponsive linear, graft, and comb‐like copolymers with azobenzene chromophores in the main‐chain and/or side‐chain are prepared via a sequential ring‐opening metathesis polymerization (ROMP) and head‐to‐tail acyclic diene metathesis (ADMET) polymerization in a one‐pot procedure using Grubbs ruthenium‐based catalysts. The diluted solutions of these as‐prepared copolymers containing azobenzene chromophores exhibit photochemical trans–cis isomerization under the irradiation of UV light, followed by their cis–trans back‐isomerization in visible light. The rates of photoisomerization are found to be slower than those of back‐isomerization, and the rate for the comb‐like copolymer is found to be from 3 to 7 times slower than that obtained for the linear or graft copolymer. This is ascribed to the differences in structure of the copolymers and the specific location of azobenzene chromophores in the copolymer, which favor a side‐chain graft structure.
Xu, Bing; Zhang, Yinyu; Liu, Wenguang
doi: 10.1002/marc.201500256pmid: 26103524
A double hydrogen bonding (DHB) hydrogel is constructed by copolymerization of 2‐vinyl‐4,6‐diamino‐1,3,5‐triazine (hydrophobic hydrogen bonding monomer) and N,N‐dimethylacrylamide (hydrophilic hydrogen bonding monomer) with polyethylene glycol diacrylates. The DHB hydrogels demonstrate tunable robust mechanical properties by varying the ratio of hydrogen bonding monomer or crosslinker. Importantly, because of synergistic energy dissipating mechanism of strong diaminotriazine (DAT) hydrogen bonding and weak amide hydrogen bonding, the DHB hydrogels exhibit high toughness (up to 2.32 kJ m−2), meanwhile maintaining 0.7 MPa tensile strength, 130% elongation at break, and 8.3 MPa compressive strength. Moreover, rehydration can help to recover the mechanical properties of the cyclic loaded–unloaded gels. Attractively, the DHB hydrogels are responsive to CO2 in water, and demonstrate unprecedented CO2‐triggered shape memory behavior owing to the reversible destruction and reconstruction of DAT hydrogen bonding upon passing and degassing CO2 without introducing external acid. The CO2 triggering mechanism may point out a new approach to fabricate shape memory hydrogels.
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