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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/28915007/synthesis-and-properties-of-2d-carbon-graphdiyne
#1
Zhiyu Jia, Yongjun Li, Zicheng Zuo, Huibiao Liu, Changshui Huang, Yuliang Li
Graphdiyne (GDY) is a flat material comprising sp(2)- and sp-hybridized carbon atoms with high degrees of π conjugation that features uniformly distributed pores. It is interesting not only from a structural point of view but also from the perspective of its electronic, chemical, mechanical, and magnetic properties. We have developed an in situ homocoupling reaction of hexaethynylbenzene on Cu foil for the fabrication of large-area ordered films of graphdiyne. These films are uniform and composed of graphdiyne multilayers...
September 15, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28915003/the-evolution-of-dna-templated-synthesis-as-a-tool-for-materials-discovery
#2
Rachel K O'Reilly, Andrew J Turberfield, Thomas R Wilks
Precise control over reactivity and molecular structure is a fundamental goal of the chemical sciences. Billions of years of evolution by natural selection have resulted in chemical systems capable of information storage, self-replication, catalysis, capture and production of light, and even cognition. In all these cases, control over molecular structure is required to achieve a particular function: without structural control, function may be impaired, unpredictable, or impossible. The search for molecules with a desired function is often achieved by synthesizing a combinatorial library, which contains many or all possible combinations of a set of chemical building blocks (BBs), and then screening this library to identify "successful" structures...
September 15, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28915001/design-of-donor-polymers-with-strong-temperature-dependent-aggregation-property-for-efficient-organic-photovoltaics
#3
Huawei Hu, Philip C Y Chow, Guangye Zhang, Tingxuan Ma, Jing Liu, Guofang Yang, He Yan
Bulk heterojunction (BHJ) organic solar cells (OSCs) have attracted intensive research attention over the past two decades owing to their unique advantages including mechanical flexibility, light weight, large area, and low-cost fabrications. To date, OSC devices have achieved power conversion efficiencies (PCEs) exceeding 12%. Much of the progress was enabled by the development of high-performance donor polymers with favorable morphological, electronic, and optical properties. A key problem in morphology control of OSCs is the trade-off between achieving small domain size and high polymer crystallinity, which is especially important for the realization of efficient thick-film devices with high fill factors...
September 15, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28910080/cell-surface-interactions-on-arginine-rich-cell-penetrating-peptides-allow-for-multiplex-modes-of-internalization
#4
Shiroh Futaki, Ikuhiko Nakase
One of the recent hot topics in peptide-related chemical biology research is the potential of cell-penetrating peptides (CPPs). Owing to their ability to deliver exogenous molecules into cells easily and effectively, their flexible design that allows transporters to comprise various chemical structures and functions, and their potential in chemical and cell biology studies and clinical applications, CPPs have been attracting enormous interest among researchers in related fields. Consequently, publications on CPPs have increased significantly...
September 14, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28902990/high-purity-semiconducting-single-walled-carbon-nanotubes-a-key-enabling-material-in-emerging-electronics
#5
Jacques Lefebvre, Jianfu Ding, Zhao Li, Paul Finnie, Gregory Lopinski, Patrick R L Malenfant
Semiconducting single-walled carbon nanotubes (sc-SWCNTs) are emerging as a promising material for high-performance, high-density devices as well as low-cost, large-area macroelectronics produced via additive manufacturing methods such as roll-to-roll printing. Proof-of-concept demonstrations have indicated the potential of sc-SWCNTs for digital electronics, radiofrequency circuits, radiation hard memory, improved sensors, and flexible, stretchable, conformable electronics. Advances toward commercial applications bring numerous opportunities in SWCNT materials development and characterization as well as fabrication processes and printing technologies...
September 13, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28891639/three-principles-of-diversity-generating-biosynthesis
#6
Wenjia Gu, Eric W Schmidt
Natural products are significant therapeutic agents and valuable drug leads. This is likely owing to their three-dimensional structural complexity, which enables them to form complex interactions with biological targets. Enzymes from natural product biosynthetic pathways show great potential to generate natural product-like compounds and libraries. Many challenges still remain in biosynthesis, such as how to rationally synthesize small molecules with novel structures and how to generate maximum chemical diversity...
September 11, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28891636/cuaac-based-click-chemistry-in-self-healing-polymers
#7
Diana Döhler, Philipp Michael, Wolfgang H Binder
Click chemistry has emerged as a significant tool for materials science, organic chemistry, and bioscience. Based on the initial concept of Barry Sharpless in 2001, the copper(I)-catalyzed azide/alkyne cycloaddition (CuAAC) reaction has triggered a plethora of chemical concepts for linking molecules and building blocks under ambient conditions, forming the basis for applications in autonomous cross-linking materials. Self-healing systems on the other hand are often based on mild cross-linking chemistries that are able to react either autonomously or upon an external trigger...
September 11, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28885830/oligoprolines-as-molecular-entities-for-controlling-distance-in-biological-and-material-sciences
#8
Stefanie Dobitz, Matthew R Aronoff, Helma Wennemers
Nature utilizes large biomolecules to fulfill tasks that require spatially well-defined arrangements at the molecular level such as electron transfer, ligand-receptor interactions, or catalysis. The creation of synthetic molecules that enable precise control over spacing and functionalization provides opportunities across diverse disciplines. Key requirements of functionalizable oligomeric scaffolds include the specific control of their molecular properties where the correct balance of flexibility and rigidity must be maintained in addition to the prerequisite of defined length...
September 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28880530/novel-in-situ-techniques-for-studies-of-model-catalysts
#9
Edvin Lundgren, Chu Zhang, Lindsay R Merte, Mikhail Shipilin, Sara Blomberg, Uta Hejral, Jianfeng Zhou, Johan Zetterberg, Johan Gustafson
Motivated mainly by catalysis, gas-surface interaction between single crystal surfaces and molecules has been studied for decades. Most of these studies have been performed in well-controlled environments and have been instrumental for the present day understanding of catalysis, providing information on surface structures, adsorption sites, and adsorption and desorption energies relevant for catalysis. However, the approach has been criticized for being too far from a catalyst operating under industrial conditions at high temperatures and pressures...
September 7, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28876890/bioorthogonal-cycloadditions-computational-analysis-with-the-distortion-interaction-model-and-predictions-of-reactivities
#10
Fang Liu, Yong Liang, K N Houk
Bioorthogonal chemistry has had a major impact on the study of biological processes in vivo. Biomolecules of interest can be tracked by using probes and reporters that do not react with cellular components and do not interfere with metabolic processes in living cells. Much time and effort has been devoted to the screening of potential bioorthogonal reagents experimentally. This Account describes how our groups have performed computational screening of reactivity and mutual orthogonality. Our collaborations with experimentalists have led to the development of new and useful reactions...
September 6, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28876055/supramolecular-assembly-of-peptide-amphiphiles
#11
Mark P Hendricks, Kohei Sato, Liam C Palmer, Samuel I Stupp
Peptide amphiphiles (PAs) are small molecules that contain hydrophobic components covalently conjugated to peptides. In this Account, we describe recent advances involving PAs that consist of a short peptide sequence linked to an aliphatic tail. The peptide sequence can be designed to form β-sheets among the amino acids near the alkyl tail, while the residues farthest from the tail are charged to promote solubility and in some cases contain a bioactive sequence. In water, β-sheet formation and hydrophobic collapse of the aliphatic tails induce assembly of the molecules into supramolecular one-dimensional nanostructures, commonly high-aspect-ratio cylindrical or ribbonlike nanofibers...
September 6, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28876046/electron-bifurcation-thermodynamics-and-kinetics-of-two-electron-brokering-in-biological-redox-chemistry
#12
Peng Zhang, Jonathon L Yuly, Carolyn E Lubner, David W Mulder, Paul W King, John W Peters, David N Beratan
How can proteins drive two electrons from a redox active donor onto two acceptors at very different potentials and distances? And how can this transaction be conducted without dissipating very much energy or violating the laws of thermodynamics? Nature appears to have addressed these challenges by coupling thermodynamically uphill and downhill electron transfer reactions, using two-electron donor cofactors that have very different potentials for the removal of the first and second electron. Although electron bifurcation is carried out with near perfection from the standpoint of energy conservation and electron delivery yields, it is a biological energy transduction paradigm that has only come into focus recently...
September 6, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28872834/the-curious-case-of-fluorination-of-conjugated-polymers-for-solar-cells
#13
Qianqian Zhang, Mary Allison Kelly, Nicole Bauer, Wei You
Organic solar cells (OSCs) have been a rising star in the field of renewable energy since the introduction of the bulk heterojunction (BHJ) in 1992. Recent advances have pushed the efficiencies of OSCs to over 13%, an impressive accomplishment via collaborative efforts in rational materials design and synthesis, careful device engineering, and fundamental understanding of device physics. Throughout these endeavors, several design principles for the conjugated donor polymers used in such solar cells have emerged, including optimizing the conjugated backbone with judicious selection of building blocks, side-chain engineering, and substituents...
September 5, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28872829/guest-responsive-metal-organic-frameworks-as-scaffolds-for-separation-and-sensing-applications
#14
Avishek Karmakar, Partha Samanta, Aamod V Desai, Sujit K Ghosh
Metal-organic frameworks (MOFs) have evolved to be next-generation utility materials because of their serviceability in a wide variety of applications. Built from organic ligands with multiple binding sites in conjunction with metal ions/clusters, these materials have found profound advantages over their other congeners in the domain of porous materials. The plethora of applications that these materials encompass has motivated material chemists to develop such novel materials, and the catalogue of MOFs is thus ever-escalating...
September 5, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28872827/rare-earth-polyoxometalates
#15
Colette Boskovic
Longstanding and important applications make use of the chemical and physical properties of both rare earth metals and polyoxometalates of early transition metals. The catalytic, optical, and magnetic features of rare earth metal ions are well-known, as are the reversible multielectron redox and photoredox capabilities of polyoxomolybdates and polyoxotungstates. The combination of rare earth ions and polyoxometalates in discrete molecules and coordination polymers is of interest for the unique combination of chemical and physical properties that can arise...
September 5, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28872296/development-of-selective-peptide-catalysts-with-secondary-structural-frameworks
#16
Kengo Akagawa, Kazuaki Kudo
Enzymes are biogenic catalysts that enable the vital activity of organisms. Enzymes promote reactions in a selective manner with a high level of substrate recognition ability. The development of such a sophisticated catalyst has been one of the goals for chemists. A synthetic peptide is the prime candidate to realize an enzyme-like catalyst. Considering that the catalytic function of enzymes derives from their molecular structures, the key for the creation of a peptide catalyst might be the introduction of a specific three-dimensional structure...
September 5, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28862837/silver-clusters-in-zeolites-from-self-assembly-to-ground-breaking-luminescent-properties
#17
Eduardo Coutiño-Gonzalez, Wouter Baekelant, Julian A Steele, Cheol Woong Kim, Maarten B J Roeffaers, Johan Hofkens
Interest for functional silver clusters (Ag-CLs) has rapidly grown over years due to large advances in the field of nanoscale fabrication and materials science. The continuous development of strategies to fabricate small-scale silver clusters, together with their interesting physicochemical properties (molecule-like discrete energy levels, for example), make them very attractive for a wide variety of applied research fields, from biotechnology and the environmental sciences to fundamental chemistry and physics...
September 1, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28862427/clay-water-and-salt-controls-on-the-permeability-of-fine-grained-sedimentary-rocks
#18
Ian C Bourg, Jonathan B Ajo-Franklin
The ability to predict the permeability of fine-grained soils, sediments, and sedimentary rocks is a fundamental challenge in the geosciences with potentially transformative implications in subsurface hydrology. In particular, fine-grained sedimentary rocks (shale, mudstone) constitute about two-thirds of the sedimentary rock mass and play important roles in three energy technologies: petroleum geology, geologic carbon sequestration, and radioactive waste management. The problem is a challenging one that requires understanding the properties of complex natural porous media on several length scales...
September 1, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28858480/anodic-cyclization-reactions-and-the-mechanistic-strategies-that-enable-optimization
#19
Ruozhu Feng, Jake A Smith, Kevin D Moeller
Oxidation reactions are powerful tools for synthesis because they allow us to reverse the polarity of electron-rich functional groups, generate highly reactive intermediates, and increase the functionality of molecules. For this reason, oxidation reactions have been and continue to be the subject of intense study. Central to these efforts is the development of mechanism-based strategies that allow us to think about the reactive intermediates that are frequently central to the success of the reactions and the mechanistic pathways that those intermediates trigger...
August 31, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28849912/synthesis-and-applications-of-boronate-affinity-materials-from-class-selectivity-to-biomimetic-specificity
#20
Zhen Liu, Hui He
Due to the complexity of biological systems and samples, specific capture and targeting of certain biomolecules is critical in much biological research and many applications. cis-Diol-containing biomolecules, a large family of important compounds including glycoproteins, saccharides, nucleosides, nucleotides, and so on, play essential roles in biological systems. As boronic acids can reversibly bind with cis-diols, boronate affinity materials (BAMs) have gained increasing attention in recent years. However, real-world applications of BAMs are often severely hampered by three bottleneck issues, including nonbiocompatible binding pH, weak affinity, and difficulty in selectivity manipulation...
August 29, 2017: Accounts of Chemical Research
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