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ACS Central Science

Fei Wang, Xiulin Fan, Tao Gao, Wei Sun, Zhaohui Ma, Chongyin Yang, Fudong Han, Kang Xu, Chunsheng Wang
Nonaqueous rechargeable magnesium (Mg) batteries suffer from the complicated and moisture-sensitive electrolyte chemistry. Besides electrolytes, the practicality of a Mg battery is also confined by the absence of high-performance electrode materials due to the intrinsically slow Mg(2+) diffusion in the solids. In this work, we demonstrated a rechargeable aqueous magnesium ion battery (AMIB) concept of high energy density, fast kinetics, and reversibility. Using a superconcentration approach we expanded the electrochemical stability window of the aqueous electrolyte to 2...
October 25, 2017: ACS Central Science
Thomas Vidil, Nicholas Hampu, Marc A Hillmyer
A lamellar diblock polymer combining a cross-linkable segment with a chemically etchable segment was cross-linked above its order-disorder temperature (TODT) to kinetically trap the morphology associated with the fluctuating disordered state. After removal of the etchable block, evaluation of the resulting porous thermoset allows for an unprecedented experimental characterization of the trapped disordered phase. Through a combination of small-angle X-ray scattering, nitrogen sorption, scanning electron microscopy, and electron tomography experiments we demonstrate that the nanoporous structure exhibits a narrow pore size distribution and a high surface to volume ratio and is bicontinuous over a large sample area...
October 25, 2017: ACS Central Science
Bowen Liu, Bharath Ramsundar, Prasad Kawthekar, Jade Shi, Joseph Gomes, Quang Luu Nguyen, Stephen Ho, Jack Sloane, Paul Wender, Vijay Pande
We describe a fully data driven model that learns to perform a retrosynthetic reaction prediction task, which is treated as a sequence-to-sequence mapping problem. The end-to-end trained model has an encoder-decoder architecture that consists of two recurrent neural networks, which has previously shown great success in solving other sequence-to-sequence prediction tasks such as machine translation. The model is trained on 50,000 experimental reaction examples from the United States patent literature, which span 10 broad reaction types that are commonly used by medicinal chemists...
October 25, 2017: ACS Central Science
Wayne Lin, Catherine J Murphy
Photothermal desorption of molecules from plasmonic nanoparticles is an example of a light-triggered molecular release due to heating of the system. However, this phenomenon ought to work only if the molecule-nanoparticle interaction is exothermic in nature. In this study, we compare protein adsorption behavior onto gold nanoparticles for both endothermic and exothermic complexation reactions, and demonstrate that Le Chatelier's principle can be applied to predict protein adsorption or desorption on nanomaterial surfaces...
October 25, 2017: ACS Central Science
Stéphanie Valleau, Romain A Studer, Florian Häse, Christoph Kreisbeck, Rafael G Saer, Robert E Blankenship, Eugene I Shakhnovich, Alán Aspuru-Guzik
We present a study on the evolution of the Fenna-Matthews-Olson bacterial photosynthetic pigment-protein complex. This protein complex functions as an antenna. It transports absorbed photons-excitons-to a reaction center where photosynthetic reactions initiate. The efficiency of exciton transport is therefore fundamental for the photosynthetic bacterium's survival. We have reconstructed an ancestor of the complex to establish whether coherence in the exciton transport was selected for or optimized over time...
October 25, 2017: ACS Central Science
Lingfei Zeng, Wen-Horng Wang, Justine Arrington, Gengbao Shao, Robert L Geahlen, Chang-Deng Hu, W Andy Tao
Protein kinases and their substrates comprise extensive signaling networks that regulate many diverse cellular functions. However, methods and techniques to systematically identify kinases directly responsible for specific phosphorylation events have remained elusive. Here we describe a novel proteomic strategy termed fluorescence complementation mass spectrometry (FCMS) to identify kinase-substrate pairs in high throughput. The FCMS strategy employs a specific substrate and a kinase library, both of which are fused with fluorescence complemented protein fragments...
October 25, 2017: ACS Central Science
Timothy W Bumpus, Jeremy M Baskin
Chemical imaging techniques have played instrumental roles in dissecting the spatiotemporal regulation of signal transduction pathways. Phospholipase D (PLD) enzymes affect cell signaling by producing the pleiotropic lipid second messenger phosphatidic acid via hydrolysis of phosphatidylcholine. It remains a mystery how this one lipid signal can cause such diverse physiological and pathological signaling outcomes, due in large part to a lack of suitable tools for visualizing the spatial and temporal dynamics of its production within cells...
October 25, 2017: ACS Central Science
Arumugam Manthiram
Lithium ion batteries as a power source are dominating in portable electronics, penetrating the electric vehicle market, and on the verge of entering the utility market for grid-energy storage. Depending on the application, trade-offs among the various performance parameters-energy, power, cycle life, cost, safety, and environmental impact-are often needed, which are linked to severe materials chemistry challenges. The current lithium ion battery technology is based on insertion-reaction electrodes and organic liquid electrolytes...
October 25, 2017: ACS Central Science
Joaquín Barroso-Flores
No abstract text is available yet for this article.
October 25, 2017: ACS Central Science
Sarah Webb
No abstract text is available yet for this article.
October 25, 2017: ACS Central Science
Michael Torrice
No abstract text is available yet for this article.
October 25, 2017: ACS Central Science
Carolyn Bertozzi
No abstract text is available yet for this article.
October 25, 2017: ACS Central Science
Anouck M Champsaur, Jaeeun Yu, Xavier Roy, Daniel W Paley, Michael L Steigerwald, Colin Nuckolls, Christopher M Bejger
We describe a new approach to synthesize two-dimensional (2D) nanosheets from the bottom-up. We functionalize redox-active superatoms with groups that can direct their assembly into multidimensional solids. We synthesized Co6Se8[PEt2(4-C6H4COOH)]6 and found that it forms a crystalline assembly. The solid-state structure is a three-dimensional (3D) network in which the carboxylic acids form intercluster hydrogen bonds. We modify the self-assembly by replacing the reversible hydrogen bonds that hold the superatoms together with zinc carboxylate bonds via the solvothermal reaction of Co6Se8[PEt2(4-C6H4COOH)]6 with Zn(NO3)2...
September 27, 2017: ACS Central Science
Natan-Haim Kalson, David Furman, Yehuda Zeiri
Despite decades of research, how life began on Earth remains one of the most challenging scientific conundrums facing modern science. It is agreed that the first step was synthesis of organic compounds essential to obtain amino acids and their polymers. Several possible scenarios that could accomplish this step, using simple inorganic molecules, have been suggested and studied over the years. The present study examines, using atomistic reactive molecular dynamics simulations, the long-standing suggestion that natural cavitation in primordial oceans was a dominant mechanism of organic molecule synthesis...
September 27, 2017: ACS Central Science
Ming Gong, Zhi Cao, Wei Liu, Eva M Nichols, Peter T Smith, Jeffrey S Derrick, Yi-Sheng Liu, Jinjia Liu, Xiaodong Wen, Christopher J Chang
Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1...
September 27, 2017: ACS Central Science
Anna Paula V Moura, Luiza C B Santos, Carlos Ramon Nascimento Brito, Edward Valencia, Caroline Junqueira, Adalberto A P Filho, Mauricio R V Sant'Anna, Nelder F Gontijo, Daniella C Bartholomeu, Ricardo T Fujiwara, Ricardo T Gazzinelli, Craig S McKay, Carlos A Sanhueza, M G Finn, Alexandre Ferreira Marques
Secreted and surface-displayed carbohydrates are essential for virulence and viability of many parasites, including for immune system evasion. We have identified the α-Gal trisaccharide epitope on the surface of the protozoan parasites Leishmania infantum and Leishmania amazonensis, the etiological agents of visceral and cutaneous leishmaniasis, respectively, with the latter bearing larger amounts of α-Gal than the former. A polyvalent α-Gal conjugate on the immunogenic Qβ virus-like particle was tested as a vaccine against Leishmania infection in a C57BL/6 α-galactosyltransferase knockout mouse model, which mimics human hosts in producing high titers of anti-α-Gal antibodies...
September 27, 2017: ACS Central Science
Jingjing Qiu, Hamed Hajibabaei, Michael R Nellist, Forrest A L Laskowski, Thomas W Hamann, Shannon W Boettcher
Electrocatalysts improve the efficiency of light-absorbing semiconductor photoanodes driving the oxygen evolution reaction, but the precise function(s) of the electrocatalysts remains unclear. We directly measure, for the first time, the interface carrier transport properties of a prototypical visible-light-absorbing semiconductor, α-Fe2O3, in contact with one of the fastest known water oxidation catalysts, Ni0.8Fe0.2O x , by directly measuring/controlling the current and/or voltage at the Ni0.8Fe0.2O x catalyst layer using a second working electrode...
September 27, 2017: ACS Central Science
Martin G Strebl, Arthur J Campbell, Wen-Ning Zhao, Frederick A Schroeder, Misha M Riley, Peter S Chindavong, Thomas M Morin, Stephen J Haggarty, Florence F Wagner, Tobias Ritter, Jacob M Hooker
Histone deacetylase 6 (HDAC6) function and dysregulation have been implicated in the etiology of certain cancers and more recently in central nervous system (CNS) disorders including Rett syndrome, Alzheimer's and Parkinson's diseases, and major depressive disorder. HDAC6-selective inhibitors have therapeutic potential, but in the CNS drug space the development of highly brain penetrant HDAC inhibitors has been a persistent challenge. Moreover, no tool exists to directly characterize HDAC6 and its related biology in the living human brain...
September 27, 2017: ACS Central Science
Antonio Fernandez, Matthieu Vermeren, Duncan Humphries, Ramon Subiros-Funosas, Nicole Barth, Lara Campana, Alison MacKinnon, Yi Feng, Marc Vendrell
Immunomodulatory agents represent one of the most promising strategies for enhancing tissue regeneration without the side effects of traditional drug-based therapies. Tissue repair depends largely on macrophages, making them ideal targets for proregenerative therapies. However, given the multiple roles of macrophages in tissue homeostasis, small molecule drugs must be only active in very specific subpopulations. In this work, we have developed the first prodrug-fluorophore conjugates able to discriminate closely related subpopulations of macrophages (i...
September 27, 2017: ACS Central Science
Yuecheng Zhou, Bo Li, Songsong Li, Herdeline Ann M Ardoña, William L Wilson, John D Tovar, Charles M Schroeder
Advances in supramolecular assembly have enabled the design and synthesis of functional materials with well-defined structures across multiple length scales. Biopolymer-synthetic hybrid materials can assemble into supramolecular structures with a broad range of structural and functional diversity through precisely controlled noncovalent interactions between subunits. Despite recent progress, there is a need to understand the mechanisms underlying the assembly of biohybrid/synthetic molecular building blocks, which ultimately control the emergent properties of hierarchical assemblies...
September 27, 2017: ACS Central Science
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