4,807 results match your criteria Accounts Of Chemical Research[Journal]

Complex Composites Built through Freezing.

Acc Chem Res 2022 May 19. Epub 2022 May 19.

Université de Lyon, INSA Lyon, Université Claude Bernard Lyon 1, CNRS, MATEIS UMR 5510, 69621 Villeurbanne, France.

ConspectusUsing a limited selection of ordinary components and at ambient temperature, nature has managed to produce a wide range of incredibly diverse materials with astonishingly elegant and complex architectures. Probably the most famous example is nacre, or mother-of-pearl, the inner lining of the shells of abalone and certain other mollusks. Nacre is 95% aragonite, a hard but brittle calcium carbonate mineral, that exhibits fracture toughness exceedingly greater than that of pure aragonite, when tested in the direction perpendicular to the platelets. Read More

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Zirconium Metal-Organic Cages: Synthesis and Applications.

Acc Chem Res 2022 May 17. Epub 2022 May 17.

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, 155 Yangqiao Road, West Fuzhou 350002, P.R. China.

ConspectusFor the last two decades, materials scientists have contributed to a growing library of porous crystalline materials. These synthetic materials are typically extended networks, including metal-organic frameworks (MOFs) and covalent organic frameworks (COFs), or discrete materials like metal-organic cages (MOCs) and porous organic cages (POCs). Advanced porous materials have shown promise for various applications due to their modular nature and structural tunability. Read More

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Sustainability and Polyesters: Beyond Metals and Monomers to Function and Fate.

Acc Chem Res 2022 May 17. Epub 2022 May 17.

Department of Materials, School of Natural Sciences, University of Manchester, Manchester M1 3BB, United Kingdom.

ConspectusPoor waste management and unchecked consumption underpin our current paradigm of plastics use, which is demonstrably unsustainable in the long term. Nonetheless, the utility and versatility of plastics suggest that the notion of a plastic-free society is also unsustainable. Responses to this conundrum are increasing, and among these are research efforts focused on the development of more sustainable plastics. Read More

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Self-Assembly of Nanowires: From Dynamic Monitoring to Precision Control.

Acc Chem Res 2022 May 17. Epub 2022 May 17.

Institute of Innovative Materials (I2M), Department of Materials Science and Engineering, Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, China.

ConspectusNatural biomaterials often show ordered nanowire structures (ONWS) which display unique structural color or superior mechanical performance. Meanwhile, plenty of modern nanodevices with ONWS have flourished with activities focused on both basic and applied research. Manipulating synthetic nanowire (NW) from a disordered state to a hierarchically ordered structure via various assembly strategies brings about intriguing and exotic chemical/physical properties. Read More

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Polymer-Tethered Nanoparticles: From Surface Engineering to Directional Self-Assembly.

Acc Chem Res 2022 May 16. Epub 2022 May 16.

Department of Chemistry, University of Toronto, Toronto, M5S3H6 ON, Canada.

ConspectusCurrent interest in nanoparticle ensembles is motivated by their collective synergetic properties that are distinct from or better than those of individual nanoparticles and their bulk counterparts. These new advanced optical, electronic, magnetic, and catalytic properties can find applications in advanced nanomaterials and functional devices, if control is achieved over nanoparticle organization. Self-assembly offers a cost-efficient approach to produce ensembles of nanoparticles with well-defined and predictable structures. Read More

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Bioinspired Superspreading Surface: From Essential Mechanism to Application.

Acc Chem Res 2022 May 15. Epub 2022 May 15.

Key Laboratory of Bioinspired Smart Interfacial Science, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.

ConspectusThe dynamic behavior of liquids on surfaces is ubiquitous in nature and has aroused wide attention from researchers. Among them, the superspreading surface has been extensively investigated and applied in areas ranging from film fabrication to antibiofouling, separation, etc. However, the traditional equilibrium contact angle (CA) at the thermodynamic steady-state cannot completely depict the dynamic spreading process of liquids, because the performance of these surfaces is controlled not only by the final steady superhydrophilicity (CA < 5°) but also by the superspreading speed of liquids with a CA of ∼0°. Read More

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Degradable Vinyl Polymers for Combating Marine Biofouling.

Acc Chem Res 2022 May 11. Epub 2022 May 11.

Faculty of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China.

ConspectusMarine organisms such as barnacle larvae and spores of algae adhere to underwater surfaces leading to marine biofouling. This phenomenon has numerous adverse impacts on marine industries and maritime activities. Due to the diversity of fouling organisms and the complexity of the marine environment, it is a huge challenge to combat marine biofouling, which limits the development and utilization of marine resources. Read More

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Molecular Spatiomics by Proximity Labeling.

Acc Chem Res 2022 May 5;55(10):1411-1422. Epub 2022 May 5.

Department of Chemistry, Seoul National University, Seoul 08826, Korea.

ConspectusProximity labeling can be defined as an enzymatic "in-cell" chemical reaction that catalyzes the proximity-dependent modification of biomolecules in live cells. Since the modified proteins can be isolated and identified via mass spectrometry, this method has been successfully utilized for the characterization of local proteomes such as the sub-mitochondrial proteome and the proteome at membrane contact sites, or spatiotemporal interactome information in live cells, which are not "accessible" via conventional methods. Currently, proximity labeling techniques can be applied not only for local proteome mapping but also for profiling local RNA and DNA, in addition to showing great potential for elucidating spatial cell-cell interaction networks in live animal models. Read More

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Bioinspired Approaches to Self-Assembly of Virus-like Particles: From Molecules to Materials.

Acc Chem Res 2022 May 4;55(10):1349-1359. Epub 2022 May 4.

Department of Chemistry, Indiana University, Bloomington, Indiana 47405, United States.

ConspectusWhen viewed through the lens of materials science, nature provides a vast library of hierarchically organized structures that serve as inspiration and raw materials for new synthetic materials. The structural organization of complex bioarchitectures with advanced functions arises from the association of building blocks and is strongly supported by ubiquitous mechanisms of self-assembly, where interactions among components result in spontaneous assembly into defined structures. Viruses are exemplary, where a capsid structure, often formed from the self-assembly of many individual protein subunits, serves as a vehicle for the transport and protection of the viral genome. Read More

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Chemical Nature of Heterogeneous Electrofreezing of Supercooled Water Revealed on Polar (Pyroelectric) Surfaces.

Acc Chem Res 2022 May 3;55(10):1383-1394. Epub 2022 May 3.

Department of Molecular Chemistry and Materials Science, Weizmann Institute of Science, Rehovot 7610001, Israel.

ConspectusThe ability to control the icing temperature of supercooled water (SCW) is of supreme importance in subfields of pure and applied sciences. The ice freezing of SCW can be influenced heterogeneously by electric effects, a process known as electrofreezing. This effect was first discovered during the 19th century; however, its mechanism is still under debate. Read More

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Oligopyrrolic Cages: From Classic Molecular Constructs to Chemically Responsive Polytopic Receptors.

Acc Chem Res 2022 May 2. Epub 2022 May 2.

Department of Chemistry, The University of Texas at Austin, 105 East 24th Street Stop A 5300, Austin, Texas 78712-1224, United States.

Conspectus"Functional molecular systems", discrete and self-assembled constructs where control over molecular recognition, structure, bonding, transport, release, catalytic activity, etc., is readily achieved, are a topic of current interest. Within this broad paradigm, oligopyrrolic cages have garnered attention due to their responsive recognition features. Read More

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Chiral Posttranslational Modification to Lysine ε-Amino Groups.

Acc Chem Res 2022 May 2;55(10):1456-1466. Epub 2022 May 2.

Center for Biopharmaceuticals & Department of Drug Design of Pharmacology, Faculty of Health and Medical Sciences, University of Copenhagen, Universitetsparken 2, DK-2100 Copenhagen, Denmark.

ConspectusThe sophistication of proteomic analysis has revealed that protein lysine residues are posttranslationally modified by a variety of acyl groups. Protein lysine acetylation regulates metabolism, gene expression, and microtubule formation and has been extensively studied; however, the understanding of the biological significance of other acyl posttranslational modifications (PTMs) is still in its infancy. The acylation of lysine residues is mediated either by acyltransferase "writer" enzymes or by nonenzymatic mechanisms and hydrolase enzymes, termed "erasers", that cleave various acyl PTMs to reverse the modified state. Read More

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Dendritic Fibrous Nanosilica: Discovery, Synthesis, Formation Mechanism, Catalysis, and CO Capture-Conversion.

Acc Chem Res 2022 May 2;55(10):1395-1410. Epub 2022 May 2.

Department of Chemical Sciences (DCS), Tata Institute of Fundamental Research (TIFR), Mumbai, 400005, India.

ConspectusSilica-based mesoporous nanomaterials have been widely used for a range of applications. Although mesopore materials (such as MCM-41 and SBA-15) possess high surface area, due to their tubular pore structures, pore accessibility is restricted, which causes limitations in mass transport. A new nanosilica was needed to overcome these challenges, including better accessibility, controllable particle size, and good stability. Read More

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Photoreactive Crystals Exhibiting [2 + 2] Photocycloaddition Reaction and Dynamic Effects.

Acc Chem Res 2022 May 2;55(10):1445-1455. Epub 2022 May 2.

Department of Chemistry, National University of Singapore, 117543 Singapore.

ConspectusConducting a reaction in the solid state eliminates the usage of solvents. If such reactions are conducted in a single-crystal to single-crystal (SCSC) fashion, then structural characterization by single-crystal X-ray crystallography (SCXRD) techniques provides unequivocal structural details. Although topochemical principles govern, getting single crystals at the end of a SCSC reaction purely depends on the experimental skills of the researchers. Read More

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Distinct Coordination Chemistry of Fe(III)-Based MRI Probes.

Acc Chem Res 2022 May 28;55(10):1435-1444. Epub 2022 Apr 28.

Department of Chemistry, University at Buffalo, the State University of New York, Amherst, New York 14260, United States.

ConspectusContrast agents are used in approximately 40% of all magnetic resonance imaging (MRI) procedures to improve the quality of the images based on the distribution and dynamic clearance of the agent. To date, all clinically approved contrast agents are Gd(III) coordination complexes that serve to shorten the longitudinal (T) and transverse (T) proton relaxation times of water. Recent interest in replacing Gd with biologically relevant metal ions such as Mn or Fe has led to increased interest in the aqueous coordination chemistry of their complexes. Read More

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Bioinspired Supercharging of Photoredox Catalysis for Applications in Energy and Chemical Manufacturing.

Acc Chem Res 2022 May 26;55(10):1423-1434. Epub 2022 Apr 26.

Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.

ConspectusFor more than a decade, photoredox catalysis has been demonstrating that when photoactive catalysts are irradiated with visible light, reactions occur under milder, cheaper, and environmentally friendlier conditions. Furthermore, this methodology allows for the activation of abundant chemicals into valuable products through novel mechanisms that are otherwise inaccessible. The photoredox approach, however, has been primarily used for pharmaceutical applications, where its implementation has been highly effective, but typically with a more rudimentary understanding of the mechanisms involved in these transformations. Read More

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Nanoarchitected Tough Biological Composites from Assembled Chitinous Scaffolds.

Acc Chem Res 2022 May 25;55(10):1360-1371. Epub 2022 Apr 25.

Department of Materials Science and Engineering, University of California, Irvine, California 92697, United States.

ConspectusOver hundreds of millions of years, organisms have derived specific sets of traits in response to common selection pressures that serve as guideposts for optimal biological designs. A prime example is the evolution of toughened structures in disparate lineages within plants, invertebrates, and vertebrates. Extremely tough structures can function much like armor, battering rams, or reinforcements that enhance the ability of organisms to win competitions, find mates, acquire food, escape predation, and withstand high winds or turbulent flow. Read More

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Advanced Pt-Based Core-Shell Electrocatalysts for Fuel Cell Cathodes.

Acc Chem Res 2022 May 22;55(9):1226-1236. Epub 2022 Apr 22.

Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, United States.

ConspectusProton-exchange membrane fuel cells (PEMFCs) are highly efficient energy storage and conversion devices. Thus, the platinum group metal (PGM)-based catalysts which are the dominant choice for the PEMFCs have received extensive interest during the past couple of decades. However, the drawbacks in the existing PGM-based catalysts (i. Read More

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Toward Mechanistic Understanding of Mechanochemical Reactions Using Real-Time Monitoring.

Acc Chem Res 2022 05 21;55(9):1262-1277. Epub 2022 Apr 21.

Ruđer Bošković Institute, Bijenička c. 54, 10000 Zagreb, Croatia.

The past two decades have witnessed a rapid emergence of interest in mechanochemistry-chemical and materials reactivity achieved or sustained by the action of mechanical force-which has led to application of mechanochemistry to almost all areas of modern chemical and materials synthesis: from organic, inorganic, and organometallic chemistry to enzymatic reactions, formation of metal-organic frameworks, hybrid perovskites, and nanoparticle-based materials. The recent success of mechanochemistry by ball milling has also raised questions about the underlying mechanisms and has led to the realization that the rational development and effective harnessing of mechanochemical reactivity for cleaner and more efficient chemical manufacturing will critically depend on establishing a mechanistic understanding of these reactions. Despite their long history, the development of such a knowledge framework for mechanochemical reactions is still incomplete. Read More

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From Dynamic Superwettability to Ionic/Molecular Superfluidity.

Acc Chem Res 2022 05 21;55(9):1195-1204. Epub 2022 Apr 21.

Key Laboratory of Bio-Inspired Materials and Interfacial Science, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.

Life systems present ultralow energy consumption in high-efficiency energy conversion, information transmission, and biosynthesis. The total energy intake of the human body is about 2000 kcal/day to maintain all of our activities, which is comparable to a power of ∼100 W. The energy required for the brain to work is equivalent to ∼20 W, and the rest of the energy (∼80 W) is used for other activities. Read More

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Catalysts for the Enzymatic Lipidation of Peptides.

Acc Chem Res 2022 05 20;55(9):1313-1323. Epub 2022 Apr 20.

Department of Biochemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.

Biologically active peptides are a major growing class of drugs, but their therapeutic potential is constrained by several limitations including bioavailability and poor pharmacokinetics. The attachment of functional groups like lipids has proven to be a robust and effective strategy for improving their therapeutic potential. Biochemical and bioactivity-guided screening efforts have identified the cyanobactins as a large class of ribosomally synthesized and post-translationally modified peptides (RiPPs) that are modified with lipids. Read More

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Achieving Theory-Experiment Parity for Activity and Selectivity in Heterogeneous Catalysis Using Microkinetic Modeling.

Acc Chem Res 2022 May 20;55(9):1237-1248. Epub 2022 Apr 20.

School of Chemistry and Chemical Engineering, The Queen's University of Belfast, Belfast BT9 5AG, U.K.

ConspectusMicrokinetic modeling based on density functional theory (DFT) energies plays an essential role in heterogeneous catalysis because it reveals the fundamental chemistry for catalytic reactions and bridges the microscopic understanding from theoretical calculations and experimental observations. Microkinetic modeling requires building a set of ordinary differential equations (ODEs) based on the calculation results of thermodynamic properties of adsorbates and kinetic parameters for the reaction elementary steps. Solving a microkinetic model can extract information on catalytic chemistry, including critical reaction intermediates, reaction pathways, the surface species distribution, activity, and selectivity, thus providing vital guidelines for altering catalysts. Read More

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Carbon Shell on Active Nanocatalyst for Stable Electrocatalysis.

Acc Chem Res 2022 05 18;55(9):1278-1289. Epub 2022 Apr 18.

Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea.

Electrocatalysis is a key process for renewable energy conversion and fuel production in future energy systems. Various nanostructures have been investigated to optimize the electrocatalytic activity and realize efficient energy use. However, the long-term stability of electrocatalysts is also crucial for the sustainable and reliable operation of energy devices. Read More

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Studies of Arylboronic Acids/Esters and RSiCF Reagents: Kinetics, Speciation, and Dysfunction at the Carbanion-Ate Interface.

Acc Chem Res 2022 05 18;55(9):1324-1336. Epub 2022 Apr 18.

EaStChem, University of Edinburgh, Joseph Black Building, David Brewster Road, Edinburgh EH9 3FJ, U.K.

Reagent instability reduces the efficiency of chemical processes, and while much effort is devoted to reaction optimization, less attention is paid to the mechanistic causes of reagent decomposition. Indeed, the response is often to simply use an excess of the reagent. Two reaction classes with ubiquitous examples of this are the Suzuki-Miyaura cross-coupling of boronic acids/esters and the transfer of CF or CF from the Ruppert-Prakash reagent, TMSCF. Read More

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Beyond Steric Crowding: Dispersion Energy Donor Effects in Large Hydrocarbon Ligands.

Acc Chem Res 2022 05 15;55(9):1337-1348. Epub 2022 Apr 15.

Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States.

Interactions between sterically crowded hydrocarbon-substituted ligands are widely considered to be repulsive because of the intrusion of the electron clouds of the ligand atoms into each other's space, which results in Pauli repulsion. Nonetheless, there is another interaction between the ligands which is less widely publicized but is always present. This is the London dispersion (LD) interaction which can occur between atoms or molecules in which dipoles can be induced instantaneously, for example, between the H atoms from the ligand C-H groups. Read More

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Chemo-Enzymatic Modification of the 5' Cap To Study mRNAs.

Acc Chem Res 2022 05 14;55(9):1249-1261. Epub 2022 Apr 14.

Department of Chemistry and Pharmacy, Institute of Biochemistry Westfälische Wilhelms-Universität Münster, University of Münster, Corrensstrasse 36, 48149 Münster, Germany.

The central dogma of molecular biology hinges on messenger RNA (mRNA), which presents a blueprint of the genetic information encoded in the DNA and serves as a template for translation into proteins. In addition to its fundamental importance in basic research, this class of biomolecules has recently become the first approved Covid vaccine, underscoring its utility in medical applications.Eukaryotic mRNA is heavily processed, including the 5' cap as the primary hallmark. Read More

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Single-Molecule Mechanochemical Sensing.

Acc Chem Res 2022 05 14;55(9):1214-1225. Epub 2022 Apr 14.

Department of Chemistry & Biochemistry, Kent State University, Kent, Ohio 44242, United States.

Single-molecule mechanochemical sensing (SMMS) is a novel biosensing technique using mechanical force as a signal transduction mechanism. In the mechanochemical sensing, the chemical binding of an analyte molecule to a sensing template is converted to mechanical signals, such as tensile force, of the template. Since mechanical force can be conveniently monitored by single-molecule tools, such as optical tweezers, magnetic tweezers, or Atomic Force Microscopy, mechanochemical sensing is often carried out at the single molecule level. Read More

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NbO-Based Catalysts for the Activation of C-O and C-C Bonds in the Valorization of Waste Carbon Resources.

Acc Chem Res 2022 05 13;55(9):1301-1312. Epub 2022 Apr 13.

Shanghai Key Laboratory of Functional Materials Chemistry, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.

Escalating energy demand, the depletion of fossil fuels, and abnormal climate change are recognized as the key challenges in the 21st century. The valorization of biomass and plastic, representing the most abundant natural and man-made polymers, respectively, as alternatives to fossil fuel is one of the promising solutions to creating a carbon-neutral, waste-free society. Catalysis is an essential tool for manipulating energy transformations via bond-breaking and bond-forming principles. Read More

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Water-Soluble Tris(cyclometalated) Iridium(III) Complexes for Aqueous Electron and Energy Transfer Photochemistry.

Acc Chem Res 2022 05 12;55(9):1290-1300. Epub 2022 Apr 12.

Department of Chemistry, University of Basel, St. Johanns-Ring 19, 4056 Basel, Switzerland.

Cyclometalated iridium(III) complexes are frequently employed in organic light emitting diodes, and they are popular photocatalysts for solar energy conversion and synthetic organic chemistry. They luminesce from redox-active excited states that can have high triplet energies and long lifetimes, making them well suited for energy transfer and photoredox catalysis. Homoleptic tris(cyclometalated) iridium(III) complexes are typically very hydrophobic and do not dissolve well in polar solvents, somewhat limiting their application scope. Read More

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Programmable Morphing Hydrogels for Soft Actuators and Robots: From Structure Designs to Active Functions.

Acc Chem Res 2022 Apr 12. Epub 2022 Apr 12.

Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou 310027, China.

ConspectusNature provides abundant inspiration and elegant paradigms for the development of smart materials that can actuate, morph, and move on demand. One remarkable capacity of living organisms is to adapt their shapes or positions in response to stimuli. Programmed deformations or movements in plant organs are mainly driven by water absorption/dehydration of cells, while versatile motions of mollusks are based on contraction/extension of muscles. Read More

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