4,128 results match your criteria Accounts Of Chemical Research[Journal]


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

Acc Chem Res 2020 May 22. 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 May 22. 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 May 21. 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 May 20. 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 May 19. 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 May 18. 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 May 14. 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

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

Acc Chem Res 2020 May 13. 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 May 13. 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
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

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

Structural Insight into [NiFe] Hydrogenase Maturation by Transient Complexes between Hyp Proteins.

Acc Chem Res 2020 Apr 31;53(4):875-886. Epub 2020 Mar 31.

Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Katahira, Sendai 980-0812, Japan.

Conspectus[NiFe] hydrogenases catalyze reversible hydrogen production/consumption. The core unit of [NiFe] hydrogenase consists of a large and a small subunit. The active site of the large subunit of [NiFe] hydrogenases contains a NiFe(CN)CO cluster. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00022DOI Listing

Planar Hypercoordinate Motifs in Two-Dimensional Materials.

Acc Chem Res 2020 Apr 30;53(4):887-895. Epub 2020 Mar 30.

Department of Chemistry, University of Puerto Rico, Rio Piedras Campus, San Juan, Puerto Rico 00931, United States.

ConspectusAs one of the most important and versatile elements, carbon renders itself as one of the most fundamental and cutting-edge topics in chemistry, physics, and materials science. Many carbon-based chemical rules were established accordingly. While the tetrahedral predilection of tetracoordinate carbon has been a cornerstone of organic chemistry since 1874, almost a century later tetracoordinate carbon was found to be able to adopt planar structures known as planar tetracoordinate carbon (ptC), which are stabilized electronically by good π-acceptor (delocalization of a lone electron pair of ptC) or σ-donor (promoting electron transfer to electron-deficient bonding) substituents or mechanically by appropriate steric enforcement. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00025DOI Listing

Supramolecular Hydrogels with Tunable Chirality for Promising Biomedical Applications.

Acc Chem Res 2020 Apr 27;53(4):852-862. Epub 2020 Mar 27.

State Key Lab of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Dongchuan Road 800, 200240 Shanghai, China.

ConspectusChirality exits from molecular-level, supramolecular, and nanoscaled helical structures to the macroscopic level in biological life. Among these various levels, as the central structural motifs in living systems (e.g. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00012DOI Listing

Recent Progress in Chlorinated Organic Photovoltaic Materials.

Acc Chem Res 2020 Apr 27;53(4):822-832. Epub 2020 Mar 27.

Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Polymer Physics and Chemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.

ConspectusOver the past few years, the development of new materials has contributed to rapid increases in the power conversion efficiencies (PCEs) of organic photovoltaic (OPV) cells to over 17%, showing great potential for the commercialization of this technology in the near future. At this stage, designing new materials with superior performance and low cost simultaneously is of crucial importance. Chlorinated materials are emerging as new stars with very high PCEs, creating a molecular design trend to replace the most popular fluorinated materials. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00009DOI Listing

Electrophilic Azides for Materials Synthesis and Chemical Biology.

Acc Chem Res 2020 Apr 24;53(4):937-948. Epub 2020 Mar 24.

Department of Chemistry, University of Massachusetts Lowell, 1 University Avenue, Lowell, Massachusetts 01854, United States.

ConspectusOrganic azides are involved in a variety of useful transformations, including nitrene chemistry, reactions with nucleophiles and electrophiles, and cycloadditions. The 1,3-dipolar cycloadditions of azides constitute a major class of highly reliable and versatile reactions, as shown by the development and rapid adoption of click chemistry and bioorthogonal chemistry. Metal-catalyzed azide-alkyne cycloaddition (Cu/RuAAC), the prototypical click reaction, has found wide utility in pharmaceutical, biomedical, and materials sciences. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00046DOI Listing

Growth of Single-Layer and Multilayer Graphene on Cu/Ni Alloy Substrates.

Acc Chem Res 2020 Apr 24;53(4):800-811. Epub 2020 Mar 24.

Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea.

ConspectusGraphene, a one-atom-thick layer of carbon with a honeycomb lattice, has drawn great attention due to its outstanding properties and its various applications in electronic and photonic devices. Mechanical exfoliation has been used for preparing graphene flakes (from monolayer to multilayer with thick pieces also typically present), but with sizes limited typically to less than millimeters, its usefulness is limited. Chemical vapor deposition (CVD) has been shown to be the most effective technique for the scalable preparation of graphene films with high quality and uniformity. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00643DOI Listing

Syntheses of Complex Terpenes from Simple Polyprenyl Precursors.

Acc Chem Res 2020 Apr 23;53(4):949-961. Epub 2020 Mar 23.

Department of Chemistry, University of California-Berkeley, Berkeley, California 94720, United States.

ConspectusFrom structure elucidation and biogenesis to synthetic methodology and total synthesis, terpene natural products have profoundly influenced the development of organic chemistry. Moreover, their myriad functional attributes range from fragrance to pharmaceuticals and have had great societal impact. Ruzicka's formulation of the "biogenetic isoprene rule," a Nobel Prize winning discovery now over 80 years old, allowed for identification of higher order terpene (aka "isoprenoid") structures from simple five-carbon isoprene fragments. Read More

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http://dx.doi.org/10.1021/acs.accounts.0c00055DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7244337PMC

Cyclodextrin Metal-Organic Frameworks: From the Research Laboratory to the Marketplace.

Acc Chem Res 2020 Mar 17. Epub 2020 Mar 17.

Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113, United States.

ConspectusCyclodextrin-based metal-organic frameworks (CD-MOFs), derived from γ-cyclodextrin (γ-CD) and potassium ions, constitute a new class of porous, renewable, and edible MOFs that can be synthesized wholly from naturally occurring starting materials on a large scale. γ-CD is a symmetrical cyclic oligosaccharide, composed of eight asymmetric α-1,4-linked d-glucopyranosyl residues, which possesses a bucket-shaped cavity with an inner diameter of ∼1 nm and a depth of ∼0.8 nm. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00537DOI Listing

Exploring and Controlling the Polymorphism in Supramolecular Assemblies of Carbohydrates and Proteins.

Acc Chem Res 2020 Apr 16;53(4):740-751. Epub 2020 Mar 16.

The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University, Shanghai 200438, P. R. China.

ConspectusIn biology, polymorphism is a well-known phenomenon by which a discrete biomacromolecule can adopt multiple specific conformations in response to its environment. This term can be extended to the ability of biomacromolecules to pack into different ordered patterns. Thus, exploration and control of the polymorphism of biomacromolecules via supramolecular methods have been key steps in achieving bioinspired structures, developing bioinspired functional materials, and exploring the mechanisms of these self-assembly processes, which are models for more complex biological systems. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00552DOI Listing

Visible-Light Photocatalytic Ozonation Using Graphitic CN Catalysts: A Hydroxyl Radical Manufacturer for Wastewater Treatment.

Acc Chem Res 2020 May 11;53(5):1024-1033. Epub 2020 Mar 11.

Beijing Engineering Research Center of Process Pollution Control, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.

ConspectusPhotocatalytic ozonation (light/O/photocatalyst), an independent advanced oxidation process (AOP) proposed in 1996, has demonstrated over the past two decades its robust oxidation capacity and potential for practical wastewater treatment using sunlight and air (source of ozone). However, its development is restricted by two main issues: (i) a lack of breakthrough catalysts working under visible light (42-43% of sunlight in energy) as well as ambiguous property-activity relationships and (ii) unclear fundamental reasons underlying its high yield of hydroxyl radicals (OH). In this Account, we summarize our substantial contributions to solving these issues, including (i) new-generation graphitic carbon nitride (g-CN) catalysts with excellent performance for photocatalytic ozonation under visible light, (ii) mechanisms of charge carrier transfer and reactive oxygen species (ROS) evolution, (iii) property-activity relationships, and (iv) chemical and working stabilities of g-CN catalysts. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00624DOI Listing

Shining Visible Light on Vinyl Halides: Expanding the Horizons of Photocatalysis.

Acc Chem Res 2020 Apr 9;53(4):782-791. Epub 2020 Mar 9.

Institut für Organische Chemie, Universität Regensburg, Universitätsstrasse 31, D-93053 Regensburg, Germany.

ConspectusOver the past decade, photoredox catalysis has blossomed as a powerful methodology because of its wide applicability in sustainable free-radical-mediated processes, in which light is used as a cleaner energy source to alter the redox properties of organic molecules and to drive unique chemical transformations. Numerous examples of highly selective C-C and C-heteroatom bond formation processes have been achieved this way in an efficient and waste-reducing way. Therein, the activation of widely available organic halides via single-electron reduction has been broadly applied for organic synthesis. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00615DOI Listing

Bifunctional N-Heterocyclic Carbenes Derived from l-Pyroglutamic Acid and Their Applications in Enantioselective Organocatalysis.

Acc Chem Res 2020 03 6;53(3):690-702. Epub 2020 Mar 6.

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Molecular Recognition and Function, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, 100190 Beijing, China.

In nature, enzymes are a powerful medium for the construction of enantiomerically pure chemicals, which always inspires synthetic chemists to explore new catalysts to imitate the enzyme machinery for asymmetric transformations. Vitamin B1, a bifunctional thiazolium N-heterocyclic carbene (NHC) precursor, is the coenzyme for transketolase. In the past two decades, a series of chiral NHCs, including monocyclic, bicyclic, tetracyclic, and even bridged ones, have been synthesized and successfully utilized as efficient organocatalysts for a wide variety of asymmetric organic reactions. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00635DOI Listing

Investigating Cryptic Binding Sites by Molecular Dynamics Simulations.

Acc Chem Res 2020 03 5;53(3):654-661. Epub 2020 Mar 5.

Department of Chemistry and Institute of Structural and Molecular Biology, University College London, London WC1E 0AJ, United Kingdom.

This Account highlights recent advances and discusses major challenges in investigations of cryptic (hidden) binding sites by molecular simulations. Cryptic binding sites are not visible in protein targets crystallized without a ligand and only become visible crystallographically upon binding events. These sites have been shown to be druggable and might provide a rare opportunity to target difficult proteins. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00613DOI Listing

Hybrid Catalysts for Artificial Photosynthesis: Merging Approaches from Molecular, Materials, and Biological Catalysis.

Acc Chem Res 2020 03 3;53(3):575-587. Epub 2020 Mar 3.

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.

Increasing demand for sustainable energy sources continues to motivate the development of new catalytic processes that store intermittent energy in the form of chemical bonds. In this context, photosynthetic organisms harvest light to drive dark reactions reducing carbon dioxide, an abundant and accessible carbon source, to store solar energy in the form of glucose and other biomass feedstocks. Inspired by this biological process, the field of artificial photosynthesis aims to store renewable energy in chemical bonds spanning fuels, foods, medicines, and materials using light, water, and CO as the primary chemical feedstocks, with the added benefit of mitigating the accumulation of CO as a greenhouse gas in the atmosphere. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00619DOI Listing
March 2020
22.323 Impact Factor

P-Stereogenic Amino-Phosphines as Chiral Ligands: From Privileged Intermediates to Asymmetric Catalysis.

Acc Chem Res 2020 03 27;53(3):676-689. Epub 2020 Feb 27.

Institute for Research in Biomedicine (IRB Barcelona), The Barcelona Institute of Science and Technology (BIST), Baldiri Reixac 10, 08028 Barcelona, Spain.

Among chiral phosphines, P-stereogenic phosphines provide unparalleled activity and selectivity and have thus emerged as "state-of-the-art" ligands for asymmetric hydrogenation and other industrially relevant processes. However, the synthesis of this type of ligand implies lengthy multistep sequences, which are a hurdle for many laboratories. There is a lack of methods for the rapid construction of P-stereogenic phosphine ligands. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00633DOI Listing

A Design-to-Device Pipeline for Data-Driven Materials Discovery.

Acc Chem Res 2020 03 25;53(3):599-610. Epub 2020 Feb 25.

Cavendish Laboratory, Department of Physics, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE, U.K.

The world needs new materials to stimulate the chemical industry in key sectors of our economy: environment and sustainability, information storage, optical telecommunications, and catalysis. Yet, nearly all functional materials are still discovered by "trial-and-error", of which the lack of predictability affords a major materials bottleneck to technological innovation. The average "molecule-to-market" lead time for materials discovery is currently 20 years. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00470DOI Listing

Silver-Catalyzed Activation of Terminal Alkynes for Synthesizing Nitrogen-Containing Molecules.

Acc Chem Res 2020 03 20;53(3):662-675. Epub 2020 Feb 20.

Jilin Province Key Laboratory of Organic Functional Molecular Design & Synthesis, Department of Chemistry, Northeast Normal University, Changchun 130024, China.

Alkynes are one of the most abundant chemicals in organic chemistry, and therefore the development of catalytic reactions to transform alkynes into other useful functionalities is of great value. In recent decades, extraordinary advances have been made in this area with transition-metal catalysis, and silver-based reagents are ideal for the activation of alkynes. This high reactivity is probably due to the superior π-Lewis acidic, carbophilic behavior of silver(I), allowing it to selectively activate carbon-carbon triple bonds (C≡C) through the formation of a silver-π complex. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00623DOI Listing

Catalyzing Electrosynthesis: A Homogeneous Electrocatalytic Approach to Reaction Discovery.

Acc Chem Res 2020 03 20;53(3):547-560. Epub 2020 Feb 20.

Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York 14850, United States.

Electrochemistry has been used as a tool to drive chemical reactions for over two centuries. With the help of an electrode and a power source, chemists are bestowed with an imaginary reagent whose potential can be precisely dialed in. The theoretically infinite redox range renders electrochemistry capable of oxidizing or reducing some of the most tenacious compounds (e. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00529DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7245362PMC

Soft Nanoarchitectonics for Enantioselective Biosensing.

Acc Chem Res 2020 03 19;53(3):644-653. Epub 2020 Feb 19.

World Premier International (WPI) Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.

Chirality is a fundamental property of a molecule, and the significant progress in chirality detection and quantification of a molecule has inspired major advances in various fields ranging from chemistry, biology, to biotechnology and pharmacology. Chiral molecules have identical molecular formulas, atom-to-atom linkages, and bonding distances, and as such they are difficult to distinguish both sensitively and selectively. Today, most new drugs and those under development are chiral, which requires technological developments in the separation and detection of chiral molecules. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00612DOI Listing

Total Synthesis of Natural Products with Bridged Bicyclo[m.n.1] Ring Systems via Type II [5 + 2] Cycloaddition.

Acc Chem Res 2020 03 18;53(3):703-718. Epub 2020 Feb 18.

Shenzhen Grubbs Institute and Department of Chemistry, Southern University of Science and Technology (SUSTech), Shenzhen 518055, China.

Natural products containing bridged ring systems are widely identified and show significant biological activity. The development of efficient synthesis reactions and strategies to construct bridged ring systems is a long-standing but very significant challenge in organic chemistry. In 2014, our group developed a unique type II [5 + 2] cycloaddition reaction that provides a facile and direct methodology for constructing highly functionalized bridged bicyclo[4. Read More

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http://dx.doi.org/10.1021/acs.accounts.9b00640DOI Listing