4,149 results match your criteria Accounts of Chemical Research [Journal]


Cobalt-Catalyzed Cross-Couplings between Alkyl Halides and Grignard Reagents.

Acc Chem Res 2020 Jul 10. Epub 2020 Jul 10.

Molecular, Macromolecular Chemistry and Materials, ESPCI Paris, CNRS, PSL University, 10 rue Vauquelin, 75005 Paris, France.

ConspectusMetal-catalyzed cross-couplings have emerged as essential tools for the construction of C-C bonds. The identification of efficient catalytic systems as well as large substrate scope made these cross-couplings key reactions to access valuable molecules ranging from materials, agrochemicals to active pharmaceutical ingredients. They have been increasingly integrated in retrosynthetic plans, allowing shorter and original route development. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00238DOI Listing

New Perspectives to Trigger and Modulate Circularly Polarized Luminescence of Complex and Aggregated Systems: Energy Transfer, Photon Upconversion, Charge Transfer, and Organic Radical.

Acc Chem Res 2020 Jul 10. Epub 2020 Jul 10.

CAS Center for Excellence in Nanoscience, CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology (NCNST), No.11, ZhongGuanCun BeiYiTiao, Beijing 100190, P.R. China.

ConspectusChiral functional materials with circularly polarized luminescence (CPL) have risen rapidly in recent years because of their fascinating characteristics and potential applications in various research fields. CPL refers to the differential spontaneous emission of left (L)- and right (R)-handed circularly polarized light upon photon or electron excitation. Generally, an outstanding CPL-active material needs to possess a high luminescence dissymmetry factor () (defined as 2( - )/( + ) where is the emission intensity), which is between -2 and +2. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00112DOI Listing

Evaluating Organic Aerosol Sources and Evolution with a Combined Molecular Composition and Volatility Framework Using the Filter Inlet for Gases and Aerosols (FIGAERO).

Acc Chem Res 2020 Jul 10. Epub 2020 Jul 10.

Tofwerk, AG, Schorenstrasse 39, CH-3645 Thun, Switzerland.

ConspectusThe complex array of sources and transformations of organic carbonaceous material that comprises an important fraction of atmospheric fine particle mass, known as organic aerosol, has presented a long running challenge for accurate predictions of its abundance, distribution, and sensitivity to anthropogenic activities. Uncertainties about changes in atmospheric aerosol particle sources and abundance over time translate to uncertainties in their impact on Earth's climate and their response to changes in air quality policy. One limitation in our understanding of organic aerosol has been a lack of comprehensive measurements of its molecular composition and volatility, which can elucidate sources and processes affecting its abundance. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00259DOI Listing

N-Heterocyclic Carbenes: A Door Open to Supramolecular Organometallic Chemistry.

Acc Chem Res 2020 Jul 9. Epub 2020 Jul 9.

Institute of Advanced Materials (INAM), Centro de Innovación en Química Avanzada (ORFEO-CINQA), Universitat Jaume I, Av. Vicente Sos Baynat s/n, E-12071 Castellón, Spain.

ConspectusThe field of metallosupramolecular chemistry is clearly dominated by the use of O-, N-, and P-donor Werner-type polydentate ligands. These molecular architectures are of high interest because of their wide range of applications, which include molecular encapsulation, stabilization of reactive species, supramolecular catalysis, and drug delivery, among others. Only recently, organometallic ligands have allowed the preparation of a variety of supramolecular coordination complexes, and the term supramolecular organometallic complexes (SOCs) is gaining space within the field of metallosupramolecular chemistry. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00312DOI Listing

Oxygen-Based Anion Redox for Lithium Batteries.

Acc Chem Res 2020 Jul 7. Epub 2020 Jul 7.

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 Cass Ave, Lemont, Illinois 60439, United States.

ConspectusThe importance of current Li-ion batteries (LIBs) in modern society cannot be overstated. While the energy demands of devices increase, the corresponding enhancements in energy density of battery technologies are highly sought after. Currently, many different battery concepts, such as Li-S and metal-air among many others, have been investigated. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00104DOI Listing

Control of Physical Aging in Super-Glassy Polymer Mixed Matrix Membranes.

Acc Chem Res 2020 Jul 5. Epub 2020 Jul 5.

CSIRO Manufacturing, Private Bag 33, Clayton South MDC, VIC 3169, Australia.

ConspectusSince the discovery of polymers of intrinsic microporosity (PIMs) in 2004, the fast size-selective interconnected pore cavities of the polymers have caused the upper bound of membrane performance to be revised, twice. Simultaneously, porous materials have meant that mixed matrix membranes (MMMs) are now a relatively simple method of enhancing transport properties. While there are now reliable routes with mixed matrices to improve the fundamental transport properties of membrane materials, many of the other properties crucial for separation applications remain largely unaddressed. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00256DOI Listing

Density Functional Theory Based Methods for the Calculation of X-ray Spectroscopy.

Acc Chem Res 2020 Jul 2. Epub 2020 Jul 2.

School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom.

ConspectusThe availability of new light sources combined with the realization of the unique capabilities of spectroscopy in the X-ray region has driven tremendous advances in the field of X-ray spectroscopy. Currently, these techniques are emerging as powerful analytical tools for the study of a wide range of problems encompassing liquids, materials, and biological systems. Time-resolved measurements add a further dimension to X-ray spectroscopy, opening up the potential to resolve ultrafast chemical processes at an atomic level. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00171DOI Listing

Water Adsorption in Soft and Heterogeneous Nanopores.

Acc Chem Res 2020 Jun 29. Epub 2020 Jun 29.

Chimie ParisTech, PSL Research University, CNRS, Institut de Recherche de Chimie Paris, 75005 Paris, France.

ConspectusLiquids under confinement differ in behavior from their bulk counterparts and can acquire properties that are specific to the confined phase and linked to the nature and structure of the host matrix. While confined liquid water is not a new topic of research, the past few years have seen a series of intriguing novel features for water inside nanoscale pores. These unusual properties arise from the very specific nature of nanoporous materials, termed "soft porous crystals"; they combine large-scale flexibility with a heterogeneous internal surface. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00215DOI Listing

Metal-Organic Framework Derived Nanozymes in Biomedicine.

Acc Chem Res 2020 Jun 29. Epub 2020 Jun 29.

Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore.

ConspectusNanozymes, which integrate the advantages of both nanomaterials and natural enzymes, have accumulated enormous research interest over the past decades because of the opportunity they provide to appreciate and further cultivate artificial enzymes with comparable properties. By mimicking the coordination environments of the catalytic sites in natural enzymes, nanozymes with confined nanostructures can serve as substitutes in many catalytic processes with comparable activity and robust stability even in harsh conditions. Since the pioneering report about peroxidase-mimicking ferromagnetic nanoparticles in 2007, nanozymes have been developed as specialized for nanomaterials with intrinsic enzyme-mimicking property. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00268DOI Listing

Role of the Terrestrial Biosphere in Atmospheric Chemistry and Climate.

Acc Chem Res 2020 Jun 26. Epub 2020 Jun 26.

Climate and Space Sciences and Engineering, University of Michigan, Ann Arbor, Michigan 48109-2143, United States.

ConspectusThe terrestrial biosphere-atmosphere interface provides a key chemical, biological, and physical lower boundary for the atmosphere. The presence of vegetation itself modifies the physical boundary, or the biogeophysical aspects of the system, by controlling important climate drivers such as soil moisture, light environment, and temperature. The leaf surface area of the terrestrial biosphere provides additional surface area for emissions, and it can be up to 55% of the total Earth's surface area during the boreal summer. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00116DOI Listing

Responsive Metal Complex Probes for Time-Gated Luminescence Biosensing and Imaging.

Acc Chem Res 2020 Jun 23. Epub 2020 Jun 23.

State Key Laboratory of Fine Chemicals, Department of Chemistry, Dalian University of Technology, Dalian 116024, China.

ConspectusThe development of reliable bioanalytical probes for selective and sensitive detection of particular analytes in biological systems is essential for better understanding the roles of the analytes in their native contexts. In the last two decades, luminescent metal complexes have greatly contributed to the development of such probes for biosensing and imaging due to their unique spectral and temporal properties, controllable cell membrane permeability, and cytotoxicity. Conjugating an analyte-activatable moiety to the metal complex luminophores allows the production of responsive metal complex probes for this analyte detection. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00172DOI Listing

Polyphenol-Mediated Assembly for Particle Engineering.

Acc Chem Res 2020 Jun 22. Epub 2020 Jun 22.

ARC Centre of Excellence in Convergent Bio-Nano Science and Technology and the Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria 3010, Australia.

ConspectusPolyphenols are naturally occurring compounds that are ubiquitous in plants and display a spectrum of physical, chemical, and biological properties. For example, they are antioxidants, have therapeutic properties, absorb UV radiation, and complex with metal ions. Additionally, polyphenols display high adherence, which has been exploited for assembling nanostructured materials. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00150DOI Listing

Exploring Anion-π Interactions and Their Applications in Supramolecular Chemistry.

Acc Chem Res 2020 Jun 19. Epub 2020 Jun 19.

Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology (Ministry of Education), Department of Chemistry, Tsinghua University, Beijing 100084, China.

ConspectusNoncovalent bond interactions provide primary driving forces for supramolecular processes ranging from molecular recognition to self-assembly of sophisticated abiotic and biological machineries. While hydrogen bonding and π-π interactions are arguably textbook concepts playing indispensable parts in various scientific disciplines, noncovalent anion-π interactions have been emerging as attractive forces between π systems and negatively charged species for just about two decades. At the beginning of this century, three research groups reported independently their computational studies on the interactions between anions and aromatic compounds, proposing attractive anion-π interactions. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00243DOI Listing

The Concept of Chemical Generators: On-Site On-Demand Production of Hazardous Reagents in Continuous Flow.

Acc Chem Res 2020 Jun 16. Epub 2020 Jun 16.

Center for Continuous Flow Synthesis and Processing (CCFLOW), Research Center Pharmaceutical Engineering GmbH (RCPE), Inffeldgasse 13, 8010 Graz, Austria.

ConspectusIn recent years, a steadily growing number of chemists, from both academia and industry, have dedicated their research to the development of continuous flow processes performed in milli- or microreactors. The common availability of continuous flow equipment at virtually all scales and affordable cost has additionally impacted this trend. Furthermore, regulatory agencies such as the United States Food and Drug Administration actively encourage continuous manufacturing of active pharmaceutical ingredients (APIs) with the vision of quality and productivity improvements. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00199DOI Listing

Forging Odd-Membered Rings: Palladium-Catalyzed Asymmetric Cycloadditions of Trimethylenemethane.

Acc Chem Res 2020 Jun 11. Epub 2020 Jun 11.

Department of Chemistry, Stanford University, 333 Campus Drive, Stanford, California 94305, United States.

ConspectusThe catalytic asymmetric synthesis of complex molecules has been the focus of our research program for several decades because such strategies have significant utility for the construction of chiral building blocks for drug development as well as the total synthesis of natural products. Cycloaddition reactions are very powerful transformations in organic synthesis providing access to highly functionalized motifs from simple starting materials. In concert with this central interest, four decades ago, we reported the palladium-catalyzed trimethylenemethane (TMM) cycloaddition for forging odd-membered ring systems. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00152DOI Listing

Spray-Drying Synthesis of MOFs, COFs, and Related Composites.

Acc Chem Res 2020 Jun 4;53(6):1206-1217. Epub 2020 Jun 4.

Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and Barcelona Institute of Science and Technology, Campus UAB, Bellaterra 08193, Barcelona Spain.

ConspectusMetal-organic frameworks (MOFs) and covalent organic frameworks (COFs) are among the most attractive porous materials today. They exhibit outstanding porosity for countless applications such as gas storage, CO capture, gas separation, sensing, drug delivery, and catalysis. Moreover, researchers have recently begun to combine MOFs or COFs with other functional materials to obtain composites that boast the respective strengths, and mitigate the respective weaknesses, of each component, enabling enhanced performance in many of the aforementioned applications. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00133DOI Listing

Mechanisms of Thermal Atomic Layer Etching.

Authors:
Steven M George

Acc Chem Res 2020 Jun 1;53(6):1151-1160. Epub 2020 Jun 1.

Department of Chemistry, University of Colorado, Boulder, Colorado 80309-0215, United States.

ConspectusAtomic layer control of semiconductor processing is needed as critical dimensions are progressively reduced below the 10 nm scale. Atomic layer deposition (ALD) methods are meeting this challenge and produce conformal thin film growth on high aspect ratio features. Atomic layer etching (ALE) techniques are also required that can remove material with atomic layer precision. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00084DOI Listing

Key References: A New Feature of .

Authors:
Cynthia Burrows

Acc Chem Res 2020 Jun 29;53(6):1101. Epub 2020 May 29.

University of Utah.

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http://dx.doi.org/10.1021/acs.accounts.0c00326DOI Listing

Emerging Potassium Metal Anodes: Perspectives on Control of the Electrochemical Interfaces.

Acc Chem Res 2020 Jun 28;53(6):1161-1175. Epub 2020 May 28.

Materials Science and Engineering Program & Texas Materials Institute (TMI), The University of Texas at Austin, Austin, Texas 78712-1591, United States.

ConspectusPotassium metal serves as the anode in emerging potassium metal batteries (KMBs). It also serves as the counter electrode for potassium ion battery (KIB) half-cells, with its reliable performance being critical for assessing the working electrode material. This first-of-its-kind critical Account focuses on the dual challenge of controlling the potassium metal-substrate and the potassium metal-electrolyte interface so as to prevent dendrites. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00099DOI Listing

Synergistic Modulation of Non-Precious-Metal Electrocatalysts for Advanced Water Splitting.

Acc Chem Res 2020 Jun 28;53(6):1111-1123. Epub 2020 May 28.

Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

ConspectusHydrogen is an ideal energy carrier and plays a critical role in the future energy transition. Distinct from steam reforming, electrochemical water splitting, especially powered by renewables, has been considered as a promising technique for scalable production of high-purity hydrogen with no carbon emission. Its commercialization relies on the reduction of electricity consumption and thus hydrogen cost, calling for highly efficient and cost-effective electrocatalysts with the capability of steadily working at high hydrogen output. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00127DOI Listing

Dissolution and Precipitation Dynamics at Environmental Mineral Interfaces Imaged by In Situ Atomic Force Microscopy.

Acc Chem Res 2020 Jun 22;53(6):1196-1205. Epub 2020 May 22.

Institut für Mineralogie, University of Münster, 48149 Münster, Germany.

ConspectusChemical reactions at the mineral-solution interface control important interfacial processes, such as geochemical element cycling, nutrient recovery from eutrophicated waters, sequestration of toxic contaminants, and geological carbon storage by mineral carbonation. By time-resolved in situ imaging of nanoscale mineral interfacial reactions, it is possible to clarify the mechanisms governing mineral-fluid reactions.In this Account, we present a concise summary of this topic that addresses a current challenge at the frontier of understanding mineral interfaces and their importance to a wide range of mineral re-equilibration processes in the presence of a fluid aqueous phase. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00128DOI Listing

Intramolecularly Cross-Linked Polymers: From Structure to Function with Applications as Artificial Antibodies and Artificial Enzymes.

Acc Chem Res 2020 Jun 22;53(6):1244-1256. Epub 2020 May 22.

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

ConspectusCross-linking of polymers significantly alters their physical properties, greatly expanding their everyday utility. Indeed, the polymeric networks resulting from linkages between polymer chains are found in everyday materials from soft contact lenses and automobile tires to enamel coatings and high-performance adhesives. In contrast, intramolecularly cross-linked polymers have received far less attention until recent years, in large part because they are synthetically more challenging to prepare. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00178DOI Listing

Chemical Imaging of Surfaces with Sum Frequency Generation Vibrational Spectroscopy.

Acc Chem Res 2020 Jun 21;53(6):1139-1150. Epub 2020 May 21.

Department of Chemistry, University of Houston, Houston, Texas 77204, United States.

ConspectusSurface chemistry is a key area of study in the chemical sciences, and many system properties are dominated by the chemistry at the interface between two bulk media. While the interface may have a large influence on the system behavior, there are relatively few molecules at the interface compared to the bulk; thus, probing their unique properties has become a specialized field in physical chemistry. In addition to the heterogeneous phase chemistry, surfaces also present spatial heterogeneity (Chemistry in Two Dimensions). Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00057DOI Listing

Liquid-Liquid Phase Separation in Supermicrometer and Submicrometer Aerosol Particles.

Acc Chem Res 2020 Jun 20;53(6):1102-1110. Epub 2020 May 20.

Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.

ConspectusThe interactions of aerosol particles with light and clouds are among the most uncertain aspects of anthropogenic climate forcings. The effects of aerosol particles on climate depend on their optical properties, heterogeneous chemistry, water uptake behavior, and ice nucleation activity. These properties in turn depend on aerosol physics and chemistry including composition, size, shape, internal structure (morphology), and phase state. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00093DOI Listing

Engineering the Bio-Nano Interface Using a Multifunctional Coordinating Polymer Coating.

Acc Chem Res 2020 Jun 19;53(6):1124-1138. Epub 2020 May 19.

Department of Chemistry and Biochemistry, Florida State University, 95 Chieftan Way, Tallahassee, Florida 32306, United States.

ConspectusIn the past three decades, interest in using nanoparticles as diagnostic tools to interrogate various biosystems has witnessed remarkable growth. For instance, it has been shown that nanoparticle probes enable the study of cellular processes at the single molecule level. These advances provide new opportunities for understanding fundamental problems in biology, innovation in medicine, and the treatment of diseases. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00641DOI Listing

Efficient Occlusion of Nanoparticles within Inorganic Single Crystals.

Acc Chem Res 2020 Jun 18;53(6):1176-1186. Epub 2020 May 18.

Department of Chemistry, University of Sheffield, Brook Hill, Sheffield, South Yorkshire S3 7HF, U.K.

ConspectusIn principle, the incorporation of guest nanoparticles within host crystals should provide a straightforward and versatile route to a wide range of nanocomposite materials. However, crystallization normally involves expelling impurities, so nanoparticle occlusion is both counter-intuitive and technically challenging. Clearly, the nanoparticles should have a strong interaction with the growing crystalline lattice, but quantifying such an affinity has been challenging; the basic principles that govern efficient nanoparticle occlusion within inorganic single crystals are rather poorly understood. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00103DOI Listing

Narrowing the Band Gap: The Key to High-Performance Organic Photovoltaics.

Authors:
Pei Cheng Yang Yang

Acc Chem Res 2020 Jun 14;53(6):1218-1228. Epub 2020 May 14.

Department of Materials Science and Engineering and California NanoSystems Institute, University of California, Los Angeles, California 90095, United States.

ConspectusOrganic photovoltaics (OPVs) have attracted considerable attention in the last two decades to overcome the terawatt energy challenge and serious environmental problems. During their early development, only wide-band-gap organic semiconductors were synthesized and employed as the active layer, mainly utilizing photons in the UV-visible region and yielding power conversion efficiencies (PCEs) lower than 5%. Afterward, considerable efforts were made to narrow the polymer donor band gap in order to utilize the infrared photons, which led to the enhancement of the PCE from 5% to 12% in about a decade. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00157DOI Listing
June 2020
22.323 Impact Factor

CuH-Catalyzed Olefin Functionalization: From Hydroamination to Carbonyl Addition.

Acc Chem Res 2020 Jun 13;53(6):1229-1243. Epub 2020 May 13.

Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Ave., Cambridge, Massachusetts 02139, United States.

ConspectusIn organic synthesis, ligand-modified copper(I) hydride (CuH) complexes have become well-known reagents and catalysts for selective reduction, particularly toward Michael acceptors and carbonyl compounds. Recently, our group and others have found that these hydride complexes undergo migratory insertion (hydrocupration) with relatively unactivated and electronically unpolarized olefins, producing alkylcopper intermediates that can be leveraged to forge a variety of useful bonds. The resulting formal hydrofunctionalization reactions have formed the basis for a resurgence of research in CuH catalysis. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00164DOI Listing

Charge Transport in Zirconium-Based Metal-Organic Frameworks.

Acc Chem Res 2020 Jun 13;53(6):1187-1195. Epub 2020 May 13.

Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.

ConspectusMetal-organic frameworks (MOFs) are a class of crystalline porous materials characterized by inorganic nodes and multitopic organic linkers. Because of their molecular-scale porosity and periodic intraframework chemical functionality, MOFs are attractive scaffolds for supporting and/or organizing catalysts, photocatalysts, chemical-sensing elements, small enzymes, and numerous other functional-property-imparting, nanometer-scale objects. Notably, these objects can be installed after the synthesis of the MOF, eliminating the need for chemical and thermal compatibility of the objects with the synthesis milieu. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00106DOI Listing

Reactive VOC Production from Photochemical and Heterogeneous Reactions Occurring at the Air-Ocean Interface.

Acc Chem Res 2020 May 5;53(5):1014-1023. Epub 2020 May 5.

Department of Chemistry, University of Wisconsin, 1101 University Ave, Madison, Wisconsin 53706, United States.

ConspectusThe ocean surface serves as a source and sink for a diverse set of reactive trace gases in the atmosphere, including volatile organic compounds (VOCs), reactive halogens, and oxidized and reduced nitrogen compounds. The exchange of reactive trace gases between the atmosphere and ocean has been shown to alter atmospheric oxidant concentrations and drive particle nucleation and growth. Uncertainties in cloud radiative forcing and aerosol-cloud interactions are among the largest uncertainties in current global climate models. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00095DOI Listing

Re-examining Dust Chemical Aging and Its Impacts on Earth's Climate.

Acc Chem Res 2020 May 29;53(5):1005-1013. Epub 2020 Apr 29.

Rosenstiel School of Marine and Atmospheric Sciences, University of Miami, Miami, Florida 33149, United States.

ConspectusThe impact of atmospheric particulate matter (i.e., aerosols) on Earth's radiative balance has been and continues to be the leading source of uncertainty with respect to predictions of future temperature increases due to climate change. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00102DOI Listing

First Accounts: The Capstone of a Tenure Tour.

Authors:
Cynthia Burrows

Acc Chem Res 2020 May 29;53(5):1003-1004. Epub 2020 Apr 29.

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http://dx.doi.org/10.1021/acs.accounts.0c00227DOI Listing

Catalytic Asymmetric Reactions with -Metallated Azomethine Ylides.

Acc Chem Res 2020 May 22;53(5):1084-1100. Epub 2020 Apr 22.

College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China.

ConspectusOptically active nitrogen-containing compounds have attracted substantial attention due to their ubiquity in the cores of natural products and bioactive molecules. Among the various synthetic approaches to nitrogenous frameworks, catalytic asymmetric 1,3-dipolar cycloadditions are one of the most attractive methods because of their powerful ability to rapidly construct various chiral -heterocycles. In particular, -metallated azomethine ylides, common and readily available 1,3-dipoles, have been extensively applied in dipolar cycloaddition reactions. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00113DOI Listing
May 2020
22.323 Impact Factor

Dissecting Programmed Cell Death with Small Molecules.

Acc Chem Res 2020 May 16;53(5):1034-1045. Epub 2020 Apr 16.

Beijing National Laboratory for Molecular Sciences, Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, Synthetic and Functional Biomolecules Center, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.

ConspectusProgrammed cell death (PCD) is fundamentally an indispensable process in all cellular activities, including cell development, wound healing, and immune surveillance of tumors (Galluzzi, L. et al. 2018, 25, 486-541). Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00600DOI Listing

When Light Meets Nitrogen-Centered Radicals: From Reagents to Catalysts.

Acc Chem Res 2020 May 14;53(5):1066-1083. Epub 2020 Apr 14.

CCNU-uOttawa Joint Research Center, Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, China.

ConspectusNitrogen-centered radicals (NCRs) are a versatile class of highly reactive species that have a longer history than the classical carbon-based radicals in synthetic chemistry. Depending on the N-hybridization and substitution patterns, NCRs can serve as electrophiles or nucleophiles to undergo various radical transformations. Despite their power, progress in nitrogen-radical chemistry is still slow compared with the popularity of carbon radicals, and their considerable synthetic potential has been largely underexplored, which is, as concluded by Zard, mainly hampered by "a dearth of convenient access to these species and a lack of awareness pertaining to their reactivity". Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00090DOI Listing

Developing Scaling Relationships for Molecular Electrocatalysis through Studies of Fe-Porphyrin-Catalyzed O Reduction.

Acc Chem Res 2020 May 13;53(5):1056-1065. Epub 2020 Apr 13.

Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States.

ConspectusThe oxygen reduction reaction (ORR) is a multiproton/multielectron transformation in which dioxygen (O) is reduced to water or hydrogen peroxide and serves as the cathode reaction in most fuel cells. The ORR (O + 4e + 4H → 2HO) involves up to nine substrates and thus requires navigating a complicated reaction landscape, typically with several high-energy intermediates. Many catalysts can perform this reaction, though few operate with fast rates and at low overpotentials (close to the thermodynamic potential). Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00044DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7351079PMC
May 2020
22.323 Impact Factor

Tailored Porous Organic Polymers for Task-Specific Water Purification.

Acc Chem Res 2020 Apr 13;53(4):812-821. Epub 2020 Apr 13.

Department of Chemistry, University of South Florida, Tampa, Florida 33620, United States.

ConspectusThe Industrial Revolution has resulted in social and economic improvements, but unfortunately, with the development of manufacturing and mining, water sources have been pervaded with contaminants, putting Earth's freshwater supply in peril. Therefore, the segregation of pollutants-such as radionuclides, heavy metals, and oil spills-from water streams, has become a pertinent problem. Attempts have been made to extract these pollutants through chemical precipitation, sorbents, and membranes. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00007DOI Listing

Exploring the Chemistry of Spiroindolenines by Mechanistically-Driven Reaction Development: Asymmetric Pictet-Spengler-type Reactions and Beyond.

Acc Chem Res 2020 Apr 10;53(4):974-987. Epub 2020 Apr 10.

State Key Laboratory of Organometallic Chemistry, Center for Excellence in Molecular Synthesis, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, 345 Lingling Lu, Shanghai 200032, China.

ConspectusThe Pictet-Spengler reaction is a fundamental named reaction in organic chemistry, and it is the most straightforward method for the synthesis of tetrahydro-β-carbolines, a core structure embedded in numerous alkaloids. Spiroindolenines are often proposed as possible intermediates in Pictet-Spengler reactions. However, whether the spiroindolenine species is an intermediate in the mechanism of the asymmetric Pictet-Spengler reaction remains unclear. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00074DOI Listing

Function and Aggregation in Structural Eye Lens Crystallins.

Acc Chem Res 2020 Apr 9;53(4):863-874. Epub 2020 Apr 9.

Department of Chemistry, University of California, Irvine, California 92697-2025, United States.

ConspectusCrystallins are transparent, refractive proteins that contribute to the focusing power of the vertebrate eye lens. These proteins are extremely soluble and resist aggregation for decades, even under crowded conditions. Crystallins have evolved to avoid strong interprotein interactions and have unusual hydration properties. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00014DOI Listing

Evolution of Anion Relay Chemistry: Construction of Architecturally Complex Natural Products.

Acc Chem Res 2020 Apr 9;53(4):988-1000. Epub 2020 Apr 9.

Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, Pennsylvania 19104, United States.

Multicomponent union tactics in which three or more fragments are rapidly connected are highly prized in the construction of architecturally complex natural products. Anion Relay Chemistry (ARC), a multicomponent union tactic, has just such potential to elaborate structurally diverse scaffolds in a single operation with excellent stereochemical control. Conceptually, the ARC tactic can be divided into two main classes: "Through-Bond," by the relay of negative charge through the bonding system of a molecule; and "Through-Space," by the migration of negative charge across space by a transfer agent. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00076DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7301606PMC

Molecular Packing: Another Key Point for the Performance of Organic and Polymeric Optoelectronic Materials.

Authors:
Qianqian Li Zhen Li

Acc Chem Res 2020 Apr 3;53(4):962-973. Epub 2020 Apr 3.

Sauvage Center for Molecular Sciences, Department of Chemistry, Wuhan University, Wuhan 430072, China.

ConspectusOptoelectronic material properties are governed by the whole collective of organic moieties, and these aggregate states present the characteristic performance of extended assemblies with different molecular packing, not only of single molecules themselves. Thus, controlling molecular packing is an essential issue for obtaining the optimized optical and electronic properties. It is also a great challenge because of the unclear structures and complicated intermolecular interactions, including dispersion forces, electrostatic interactions and hydrogen bonding. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00060DOI Listing

Advances in Rhodium-Catalyzed Oxidative Arene Alkenylation.

Acc Chem Res 2020 Apr 2;53(4):920-936. Epub 2020 Apr 2.

Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, United States.

ConspectusAlkyl and alkenyl arenes are of substantial value in both large-scale and fine chemical processes. Billions of pounds of alkyl and alkenyl arenes are produced annually. Historically, the dominant method for synthesis of alkyl arenes is acid-catalyzed arene alkylation, and alkenyl arenes are often synthesized in a subsequent dehydrogenation step. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00036DOI Listing

Mechanisms of Nickel-Catalyzed Coupling Reactions and Applications in Alkene Functionalization.

Acc Chem Res 2020 Apr 2;53(4):906-919. Epub 2020 Apr 2.

Department of Chemistry, New York University, 100 Washington Square East, New York, New York 10003, United States.

ConspectusNickel complexes exhibit distinct properties from other group 10 metals, including a small nuclear radius, high paring energy, low electronegativity, and low redox potentials. These properties enable Ni catalysts to accommodate and stabilize paramagnetic intermediates, access radical pathways, and undergo slow β-H elimination. Our research program investigates how each of these fundamental attributes impact the catalytic properties of Ni, in particular in the context of alkene functionalization. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00032DOI Listing

Small-Molecule Modulators of Toll-like Receptors.

Acc Chem Res 2020 May 1;53(5):1046-1055. Epub 2020 Apr 1.

Laboratory of Chemical Biology, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin 130022, China.

ConspectusToll-like receptors (TLRs) are the "gatekeepers" of the immune system in humans and other animals to protect the host from invading bacteria, viruses, and other microorganisms. Since TLR4 was discovered as the receptor for endotoxin in the late 1990s, significant progress has been made in exploiting an understanding of the function of TLRs. The TLR-signaling pathway is crucial for the induction and progression of various diseases. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00631DOI Listing
May 2020
22.323 Impact Factor

Molecular Modeling for Artificial Metalloenzyme Design and Optimization.

Acc Chem Res 2020 Apr 1;53(4):896-905. Epub 2020 Apr 1.

Departament de Quı́mica, Universitat Autònoma de Barcelona, Edifici C.n., 08193 Cerdanyola del Vallès, Barcelona Spain.

ConspectusArtificial metalloenzymes (ArMs) are obtained by inserting homogeneous catalysts into biological scaffolds and are among the most promising strategies in the quest for new-to-nature biocatalysts. The quality of their design strongly depends on how three partners interact: the biological host, the "artificial cofactor," and the substrate. However, structural characterization of functional artificial metalloenzymes by X-ray or NMR is often partial, elusive, or absent. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00031DOI Listing

From Pd(OAc) to Chiral Catalysts: The Discovery and Development of Bifunctional Mono-N-Protected Amino Acid Ligands for Diverse C-H Functionalization Reactions.

Acc Chem Res 2020 Apr 31;53(4):833-851. Epub 2020 Mar 31.

Department of Chemistry, The Scripps Research Institute, 10550 North Torrey Pines Road, La Jolla, California 92037, United States.

ConspectusThe functionalization of unactivated carbon-hydrogen bonds is a transformative strategy for the rapid construction of molecular complexity given the ubiquitous presence of C-H bonds in organic molecules. It represents a powerful tool for accelerating the synthesis of natural products and bioactive compounds while reducing the environmental and economic costs of synthesis. At the same time, the ubiquity and strength of C-H bonds also present major challenges toward the realization of transformations that are both highly selective and efficient. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00621DOI Listing

Aromatic Heterocycles as Productive Dienophiles in the Inverse Electron-Demand Diels-Alder Reactions of 1,3,5-Triazines.

Acc Chem Res 2020 Apr 31;53(4):773-781. Epub 2020 Mar 31.

The Center for Combinatorial Chemistry and Drug Discovery of Jilin University, The School of Pharmaceutical Sciences, Jilin University, 1266 Fujin Road, Changchun, Jilin 130021, P.R. China.

ConspectusHeterocycles are often found as the structural nucleus in natural products and biological active compounds. Consequently, research toward the discovery and development of novel and efficient synthetic methodologies is of constant interest to organic chemists. Diels-Alder reactions are powerful at forming multiple bonds simultaneously, often with stereoselectivity, and thus are one of the most widely used synthetic methodologies in organic syntheses. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00604DOI Listing

Resolving Membrane Protein-Protein Interactions in Live Cells with Pulsed Interleaved Excitation Fluorescence Cross-Correlation Spectroscopy.

Acc Chem Res 2020 Apr 31;53(4):792-799. Epub 2020 Mar 31.

Department of Chemistry, University of Akron, Akron, Ohio 44325, United States.

ConspectusThe cell plasma membrane (PM) contains thousands of proteins that sense and respond to the outside environment. These proteins have evolved sensitivity to a wide variety of physical and chemical signals and act as a delivery system across the PM. Membrane proteins are critical for information flow and decision making in the cell and thus are important targets in drug development. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00625DOI Listing