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ACS Central Science

Adriana N Macedo, Stellena Mathiaparanam, Lauren Brick, Katherine Keenan, Tanja Gonska, Linda Pedder, Stephen Hill, Philip Britz-McKibbin
The sweat chloride test remains the gold standard for confirmatory diagnosis of cystic fibrosis (CF) in support of universal newborn screening programs. However, it provides ambiguous results for intermediate sweat chloride cases while not reflecting disease progression when classifying the complex CF disease spectrum given the pleiotropic effects of gene modifiers and environment. Herein we report the first characterization of the sweat metabolome from screen-positive CF infants and identify metabolites associated with disease status that complement sweat chloride testing...
August 23, 2017: ACS Central Science
Ala Bunescu, Sunwoo Lee, Qian Li, John F Hartwig
Polyolefins account for 60% of global plastic consumption, but many potential applications of polyolefins require that their properties, such as compatibility with polar polymers, adhesion, gas permeability, and surface wetting, be improved. A strategy to overcome these deficiencies would involve the introduction of polar functionalities onto the polymer chain. Here, we describe the Ni-catalyzed hydroxylation of polyethylenes (LDPE, HDPE, and LLDPE) in the presence of (m) CPBA as an oxidant. Studies with cycloalkanes and pure, long-chain alkanes were conducted to assess precisely the selectivity of the reaction and the degree to which potential C-C bond cleavage of a radical intermediate occurs...
August 23, 2017: ACS Central Science
Elvis Cudjoe, Shaghayegh Khani, Amanda E Way, Michael J A Hore, Joao Maia, Stuart J Rowan
Inspired by the ability of the sea cucumber to (reversibly) increase the stiffness of its dermis upon exposure to a stimulus, we herein report a stimuli-responsive nanocomposite that can reversibly increase its stiffness upon exposure to warm water. Nanocomposites composed of cellulose nanocrystals (CNCs) that are grafted with a lower critical solution temperature (LCST) polymer embedded within a poly(vinyl acetate) (PVAc) matrix show a dramatic increase in modulus, for example, from 1 to 350 MPa upon exposure to warm water, the hypothesis being that grafting the polymers from the CNCs disrupts the interactions between the nanofibers and minimizes the mechanical reinforcement of the film...
August 23, 2017: ACS Central Science
Hai Wang, Pranay Agarwal, Yichao Xiao, Hao Peng, Shuting Zhao, Xuanyou Liu, Shenghua Zhou, Jianrong Li, Zhenguo Liu, Xiaoming He
Stem cell therapy holds great potential for treating ischemic diseases. However, contemporary methods for local stem cell delivery suffer from poor cell survival/retention after injection. We developed a unique multiscale delivery system by encapsulating therapeutic agent-laden nanoparticles in alginate hydrogel microcapsules and further coentrapping the nano-in-micro capsules with stem cells in collagen hydrogel. The multiscale system exhibits significantly higher mechanical strength and stability than pure collagen hydrogel...
August 23, 2017: ACS Central Science
Štěpán Timr, Roman Pleskot, Jan Kadlec, Miriam Kohagen, Aniket Magarkar, Pavel Jungwirth
Recoverin is a neuronal calcium sensor involved in vision adaptation that reversibly associates with cellular membranes via its calcium-activated myristoyl switch. While experimental evidence shows that the myristoyl group significantly enhances membrane affinity of this protein, molecular details of the binding process are still under debate. Here, we present results of extensive molecular dynamics simulations of recoverin in the proximity of a phospholipid bilayer. We capture multiple events of spontaneous membrane insertion of the myristoyl moiety and confirm its critical role in the membrane binding...
August 23, 2017: ACS Central Science
Xueyan Feng, Ruimeng Zhang, Yiwen Li, You-Lee Hong, Dong Guo, Kening Lang, Kuan-Yi Wu, Mingjun Huang, Jialin Mao, Chrys Wesdemiotis, Yusuke Nishiyama, Wei Zhang, Wei Zhang, Toshikazu Miyoshi, Tao Li, Stephen Z D Cheng
To understand the hierarchical self-organization behaviors of soft materials as well as their dependence on molecular geometry, a series of AB n dendron-like molecules based on polyhedral oligomeric silsesquioxane (POSS) nanoparticles were designed and synthesized. The apex of these molecules is a hydrophilic POSS cage with 14 hydroxyl groups (denoted DPOSS). At its periphery, there are different numbers (n = 1-8) of hydrophobic POSS cages with seven isobutyl groups (denoted BPOSS), connected to the apical DPOSS via flexible dendron type linker(s)...
August 23, 2017: ACS Central Science
Zhiji Han, Ruud Kortlever, Hsiang-Yun Chen, Jonas C Peters, Theodor Agapie
Electrocatalytic CO2 reduction to generate multicarbon products is of interest for applications in artificial photosynthetic schemes. This is a particularly attractive goal for CO2 reduction by copper electrodes, where a broad range of hydrocarbon products can be generated but where selectivity for C-C coupled products relative to CH4 and H2 remains an impediment. Herein we report a simple yet highly selective catalytic system for CO2 reduction to C≥2 hydrocarbons on a polycrystalline Cu electrode in bicarbonate aqueous solution that uses N-substituted pyridinium additives...
August 23, 2017: ACS Central Science
Yueshen Wu, Jianbing Jiang, Zhe Weng, Maoyu Wang, Daniël L J Broere, Yiren Zhong, Gary W Brudvig, Zhenxing Feng, Hailiang Wang
Transition-metal-based molecular complexes are a class of catalyst materials for electrochemical CO2 reduction to CO that can be rationally designed to deliver high catalytic performance. One common mechanistic feature of these electrocatalysts developed thus far is an electrogenerated reduced metal center associated with catalytic CO2 reduction. Here we report a heterogenized zinc-porphyrin complex (zinc(II) 5,10,15,20-tetramesitylporphyrin) as an electrocatalyst that delivers a turnover frequency as high as 14...
August 23, 2017: ACS Central Science
Wenxing Wang, Peiyuan Wang, Xueting Tang, Ahmed A Elzatahry, Shuwen Wang, Daifallah Al-Dahyan, Mengyao Zhao, Chi Yao, Chin-Te Hung, Xiaohang Zhu, Tiancong Zhao, Xiaomin Li, Fan Zhang, Dongyuan Zhao
The low-efficiency cellular uptake property of current nanoparticles greatly restricts their application in the biomedical field. Herein, we demonstrate that novel virus-like mesoporous silica nanoparticles can easily be synthesized, showing greatly superior cellular uptake property. The unique virus-like mesoporous silica nanoparticles with a spiky tubular rough surface have been successfully synthesized via a novel single-micelle epitaxial growth approach in a low-concentration-surfactant oil/water biphase system...
August 23, 2017: ACS Central Science
Philipp M Cromm, Craig M Crews
As the central figure of the cellular protein degradation machinery, the proteasome is critical for cell survival. Having been extensively targeted for inhibition, the constitutive proteasome has proven its role as a highly valuable drug target. However, recent advances in the protein homeostasis field suggest that additional chapters can be added to this successful story. For example, selective immunoproteasome inhibition promises high clinical efficacy for autoimmune disorders and inflammation, and proteasome inhibitors might serve as novel therapeutics for malaria or other microorganisms...
August 23, 2017: ACS Central Science
Christopher J Welch
As the speed of chromatographic enantioseparations advances to the point where the enantiomers of most chiral compounds can be resolved in less than a minute, some in less than a second, we pose the question of how this field is likely to develop over the next few years. Are we approaching a fundamental speed limit, or will further technological advances continue to deliver faster and faster separations? Are faster separations even needed for chemical research, and if so, how will they help? We herein examine this trend, investigating the barriers that currently limit speed and offering some insights into the continued evolution of fast chromatographic enantioseparations...
August 23, 2017: ACS Central Science
Xi Zhou, Lei Ren
No abstract text is available yet for this article.
August 23, 2017: ACS Central Science
Maria M Pérez-Madrigal, Rachel K O'Reilly
No abstract text is available yet for this article.
August 23, 2017: ACS Central Science
Neil Savage
No abstract text is available yet for this article.
August 23, 2017: ACS Central Science
Louisa Dalton
No abstract text is available yet for this article.
August 23, 2017: ACS Central Science
Hung V-T Nguyen, Qixian Chen, Joseph T Paletta, Peter Harvey, Yivan Jiang, Hui Zhang, Michael D Boska, M Francesca Ottaviani, Alan Jasanoff, Andrzej Rajca, Jeremiah A Johnson
Metal-free magnetic resonance imaging (MRI) agents could overcome the established toxicity associated with metal-based agents in some patient populations and enable new modes of functional MRI in vivo. Herein, we report nitroxide-functionalized brush-arm star polymer organic radical contrast agents (BASP-ORCAs) that overcome the low contrast and poor in vivo stability associated with nitroxide-based MRI contrast agents. As a consequence of their unique nanoarchitectures, BASP-ORCAs possess per-nitroxide transverse relaxivities up to ∼44-fold greater than common nitroxides, exceptional stability in highly reducing environments, and low toxicity...
July 26, 2017: ACS Central Science
Guowu Zhan, Hua Chun Zeng
Particulate catalysts with streamline shapes have important impacts on fluid-related reactions, and they need to be properly characterized. However, utilization of streamline-shaped catalysts for heterogeneous catalysis has remained an unexplored area due to the lack of easy-to-use techniques to produce such shaped catalysts, especially at the small length scale of the submicron to micron regime. Herein, we report our recent development of a class of prototype nanocatalysts with streamline shapes. In this research, the kinetic control is adapted to obtain streamline-shaped supports, followed by functionalizing such supports with catalytically active metal nanoclusters (e...
July 26, 2017: ACS Central Science
Marta Artola, Liang Wu, Maria J Ferraz, Chi-Lin Kuo, Lluís Raich, Imogen Z Breen, Wendy A Offen, Jeroen D C Codée, Gijsbert A van der Marel, Carme Rovira, Johannes M F G Aerts, Gideon J Davies, Herman S Overkleeft
The essential biological roles played by glycosidases, coupled to the diverse therapeutic benefits of pharmacologically targeting these enzymes, provide considerable motivation for the development of new inhibitor classes. Cyclophellitol epoxides and aziridines are recently established covalent glycosidase inactivators. Inspired by the application of cyclic sulfates as electrophilic equivalents of epoxides in organic synthesis, we sought to test whether cyclophellitol cyclosulfates would similarly act as irreversible glycosidase inhibitors...
July 26, 2017: ACS Central Science
Tengfei Li, Yang Cao, Jingfu He, Curtis P Berlinguette
Electrochemical reduction of CO2 into carbon-based products using excess clean electricity is a compelling method for producing sustainable fuels while lowering CO2 emissions. Previous electrolytic CO2 reduction studies all involve dioxygen production at the anode, yet this anodic reaction requires a large overpotential and yields a product bearing no economic value. We report here that the cathodic reduction of CO2 to CO can occur in tandem with the anodic oxidation of organic substrates that bear higher economic value than dioxygen...
July 26, 2017: ACS Central Science
Masashi Mamada, Ko Inada, Takeshi Komino, William J Potscavage, Hajime Nakanotani, Chihaya Adachi
Thermally activated delayed fluorescence (TADF) materials have shown great potential for highly efficient organic light-emitting diodes (OLEDs). While the current molecular design of TADF materials primarily focuses on combining donor and acceptor units, we present a novel system based on the use of excited-state intramolecular proton transfer (ESIPT) to achieve efficient TADF without relying on the well-established donor-acceptor scheme. In an appropriately designed acridone-based compound with intramolecular hydrogen bonding, ESIPT leads to separation of the highest occupied and lowest unoccupied molecular orbitals, resulting in TADF emission with a photoluminescence quantum yield of nearly 60%...
July 26, 2017: ACS Central Science
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