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You searched for: Journal name Journal of the American Chemical Society Remove constraint Journal name: Journal of the American Chemical Society Publication year rev 7983-2017 Remove constraint Publication year rev: 7983-2017 Source 2017 v.139 no.13 Remove constraint Source: 2017 v.139 no.13
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1. Copper(I)-Catalyzed Enantioselective Addition of Enynes to Ketones

Author:
Wei Xiao-Feng; Xie Xiao-Wei; Shimizu Yohei; Kanai Motomu
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4647-4650
ISSN:
1520-5126
Subject:
alcohols; catalysts; copper; enantiomers; ketones; ligands
Abstract:
... A copper(I)-catalyzed enantioselective addition of enynes to ketones was developed. The method allows facile construction of enantiomerically enriched tertiary alcohols using skipped enynes as stable hydrocarbon pronucleophiles. The combination of a soft copper(I)-conjugated Brønsted base catalyst with a chiral diphosphine ligand, (S,S)-Ph-BPE, enabled chemoselective deprotonation of the skipped e ...
DOI:
10.1021/jacs.7b01254

2. Doubly Diastereoconvergent Preparation and Microsolvation-Controlled Properties of (Z)- and (E)-1′-Lithio-1′-(2,6-dimethylphenyl)propenes

Author:
Knorr Rudolf; Behringer Claudia; Knittl Monika; von Roman Ulrich; Lattke Ernst
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4690-4703
ISSN:
1520-5126
Subject:
ambient temperature; nuclear magnetic resonance spectroscopy; propylene; solvents
Abstract:
... A doubly diastereoconvergent reaction can ad libitum generate either one or the other of two diastereomeric products with complete consumption of the diastereomeric precorsors or their mixtures. Thus, the preparation of configurationally pure (Z)-1′-lithio-1′-(2,6-dimethylphenyl)propene [(Z)-1] from any Z,E mixture of the corresponding bromoalkenes with n-butyllithium succeeded by means of a user- ...
DOI:
10.1021/jacs.6b11003

3. Electrochemically Assisted Self-Assembly Technique for the Fabrication of Mesoporous Metal–Organic Framework Thin Films: Composition of 3D Hexagonally Packed Crystals with 2D Honeycomb-like Mesopores

Author:
Alizadeh Saber; Nematollahi Davood
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4753-4761
ISSN:
1520-5126
Subject:
crystals; electrochemistry; electrodes; electron transfer; mass transfer; porous media
Abstract:
... In this work, we introduce a novel and general strategy for the environmentally friendly fabrication of mesoporous metal–organic framework (mMOF) thin films via the electrochemically assisted self-assembly (EASA) technique. Implementation of this procedure as a one-step, additive-free, and versatile protocol leads to the in situ simultaneous synthesis and deposition of mesoporous architectures of ...
DOI:
10.1021/jacs.6b12564

4. Engineered Split-TET2 Enzyme for Inducible Epigenetic Remodeling

Author:
Lee Minjung; Li Jia; Liang Yi; Ma Guolin; Zhang Jixiang; He Lian; Liu Yuliang; Li Qian; Li Minyong; Sun Deqiang; Zhou Yubin; Huang Yun
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4659-4662
ISSN:
1520-5126
Subject:
DNA; chromatin; epigenetics; genetic code; genome; mammals; oxidation
Abstract:
... The Ten-eleven translocation (TET) family of 5-methylcytosine (5mC) dioxygenases catalyze the conversion of 5mC into 5-hydroxymethylcytosine (5hmC) and further oxidized species to promote active DNA demethylation. Here we engineered a split-TET2 enzyme to enable temporal control of 5mC oxidation and subsequent remodeling of epigenetic states in mammalian cells. We further demonstrate the use of th ...
DOI:
10.1021/jacs.7b01459
PubMed:
28294608
PubMed Central:
PMC5385525

5. Enhanced Binding Affinity for an i-Motif DNA Substrate Exhibited by a Protein Containing Nucleobase Amino Acids

Author:
Bai Xiaoguang; Talukder Poulami; Daskalova Sasha M.; Roy Basab; Chen Shengxi; Li Zhongxian; Dedkova Larisa M.; Hecht Sidney M.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4611-4614
ISSN:
1520-5126
Subject:
DNA; amino acids; binding capacity; molecular models; transcription factors; uracil
Abstract:
... Several variants of a nucleic acid binding motif (RRM1) of putative transcription factor hnRNP LL containing nucleobase amino acids at specific positions have been prepared and used to study binding affinity for the BCL2 i-motif DNA. Molecular modeling suggested a number of amino acids in RRM1 likely to be involved in interaction with the i-motif DNA, and His24 and Arg26 were chosen for modificati ...
DOI:
10.1021/jacs.6b11825
PubMed:
28263595
PubMed Central:
PMC5901667

6. Exploring Oxygen Activity in the High Energy P2-Type Na0.78Ni0.23Mn0.69O2 Cathode Material for Na-Ion Batteries

Author:
Ma Chuze; Alvarado Judith; Xu Jing; Clément Raphaële J.; Kodur Moses; Tong Wei; Grey Clare P.; Meng Ying Shirley
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4835-4845
ISSN:
1520-5126
Subject:
manganese; phase transition; research and development; energy; renewable energy sources; cathodes; X-ray absorption spectroscopy; ambient temperature; electrochemistry; sodium; nickel; oxidation; oxides; metal ions; oxygen; batteries
Abstract:
... Large-scale electric energy storage is fundamental to the use of renewable energy. Recently, research and development efforts on room-temperature sodium-ion batteries (NIBs) have been revitalized, as NIBs are considered promising, low-cost alternatives to the current Li-ion battery technology for large-scale applications. Herein, we introduce a novel layered oxide cathode material, Na₀.₇₈Ni₀.₂₃Mn₀ ...
DOI:
10.1021/jacs.7b00164

7. Light-Induced Radical Formation and Isomerization of an Aromatic Thiol in Solution Followed by Time-Resolved X-ray Absorption Spectroscopy at the Sulfur K-Edge

Author:
Ochmann Miguel; von Ahnen Inga; Cordones Amy A.; Hussain Abid; Lee Jae Hyuk; Hong Kiryong; Adamczyk Katrin; Vendrell Oriol; Kim Tae Kyu; Schoenlein Robert W.; Huse Nils
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4797-4804
ISSN:
1520-5126
Subject:
X-ray absorption spectroscopy; isomerization; isomers; lighting; models; sulfur; thiols
Abstract:
... We applied time-resolved sulfur-1s absorption spectroscopy to a model aromatic thiol system as a promising method for tracking chemical reactions in solution. Sulfur-1s absorption spectroscopy allows tracking multiple sulfur species with a time resolution of ∼70 ps at synchrotron radiation facilities. Experimental transient spectra combined with high-level electronic structure theory allow identif ...
DOI:
10.1021/jacs.6b12992

8. Lithium Metal Anodes with an Adaptive “Solid-Liquid” Interfacial Protective Layer

Author:
Liu Kai; Pei Allen; Lee Hye Ryoung; Kong Biao; Liu Nian; Lin Dingchang; Liu Yayuan; Liu Chong; Hsu Po-chun; Bao Zhenan; Cui Yi
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4815-4820
ISSN:
1520-5126
Subject:
anodes; batteries; crosslinking; electrolytes; energy density; lithium; polymers
Abstract:
... Lithium metal is an attractive anode for the next generation of high energy density lithium-ion batteries due to its high specific capacity (3,860 mAh g–¹) and lowest overall anode potential. However, the key issue is that the static solid electrolyte interphase cannot match the dynamic volume changes of the Li anode, resulting in side reactions, dendrite growth, and poor electrodeposition behavio ...
DOI:
10.1021/jacs.6b13314

9. Mechanisms of Hydrogen-Assisted CO2 Reduction on Nickel

Author:
Lin Wei; Stocker Kelsey M.; Schatz George C.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4663-4666
ISSN:
1520-5126
Subject:
carbon dioxide; catalysts; hydrogen; molecular dynamics; nickel; probability; reaction mechanisms
Abstract:
... Mechanistic details of catalytic reactions are critical to the development of improved catalysts. Here, we perform high quality Born–Oppenheimer molecular dynamics simulations of the reaction mechanisms associated with hydrogen-assisted CO₂ reduction on Ni(110). The simulation results show direct theoretical evidence for both associative and redox mechanisms in the reaction of atomic hydrogen with ...
DOI:
10.1021/jacs.7b01538

10. Mechanistic Studies of the Photoinduced Quinone Trimethyl Lock Decaging Process

Author:
Regan Clinton J.; Walton David P.; Shafaat Oliver S.; Dougherty Dennis A.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4729-4736
ISSN:
1520-5126
Subject:
absorption; electron transfer; hydrogen; isotopes; photochemistry; wavelengths
Abstract:
... Mechanistic studies of a general reaction that decages a wide range of substrates on exposure to visible light are described. The reaction involves a photochemically initiated reduction of a quinone mediated by an appended thioether. After reduction, a trimethyl lock system incorporated into the quinone leads to thermal decaging. The reaction could be viewed as an electron-transfer initiated reduc ...
DOI:
10.1021/jacs.6b12007

11. Mechanistic Studies on Rhodium-Catalyzed Enantioselective Silylation of Aryl C–H Bonds

Author:
Lee Taegyo; Hartwig John F.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4879-4886
ISSN:
1520-5126
Subject:
catalysts; chemical bonding; enantiomers; isotopes; ligands; rhodium
Abstract:
... Several classes of enantioselective silylations of C–H bonds have been reported recently, but little mechanistic data on these processes are available. We report mechanistic studies on the rhodium-catalyzed, enantioselective silylation of aryl C–H bonds. A rhodium silyl dihydride and a rhodium norbornyl complex were prepared and determined to be interconverting catalyst resting states. Kinetic iso ...
DOI:
10.1021/jacs.7b00737
PubMed:
28278372
PubMed Central:
PMC5810545

12. Nanoengineering of Core–Shell Magnetic Mesoporous Microspheres with Tunable Surface Roughness

Author:
Yue Qin; Zhang Yu; Jiang Yongjian; Li Jialuo; Zhang Hongwei; Yu Chengzhong; Elzatahry Ahmed A.; Alghamdi Abdulaziz; Deng Yonghui; Zhao Dongyuan
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4954-4961
ISSN:
1520-5126
Subject:
aqueous solutions; drugs; formaldehyde; magnetic fields; magnetic properties; nanocomposites; nanotechnology; neoplasms; petroleum; physicochemical properties; porous media; resorcinol; silica; surface area; surface roughness; therapeutics
Abstract:
... Functional core–shell mesoporous microspheres with integrated functions, controlled structure, and surface properties and morphologies have received increasing attention due to their excellent physicochemical properties. Herein, core–shell magnetic mesoporous materials with cauliflower-like morphology and tunable surface roughness have been synthesized through a kinetics-controlled interface co-as ...
DOI:
10.1021/jacs.7b01464

13. New Autoinductive Cascade for the Optical Sensing of Fluoride: Application in the Detection of Phosphoryl Fluoride Nerve Agents

Author:
Sun Xiaolong; Dahlhauser Samuel D.; Anslyn Eric V.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4635-4638
ISSN:
1520-5126
Subject:
fluorescent dyes; fluorides; nerve agents; standard operating procedures
Abstract:
... A new autoinductive cascade employing benzoyl fluoride as a latent source of fluoride is reported for signal amplification and optical detection of fluoride. The autoinduction leads to a maximum 4-fold signal enhancement for each fluoride generated, as well as a self-propagating cycle that generates three fluorophores for each single fluoride released. A two-step integrated protocol creates a more ...
DOI:
10.1021/jacs.7b01008

14. Shock Wave Chemistry in a Metal–Organic Framework

Author:
Su Zhi; Shaw William L.; Miao Yu-Run; You Sizhu; Dlott Dana D.; Suslick Kenneth S.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4619-4622
ISSN:
1520-5126
Subject:
chemical bonding; coordination polymers; endothermy; energy; spectroscopy; water power
Abstract:
... Metal–organic frameworks (MOFs) have potential applications as energy absorbing materials for shock wave energy mitigation due to their nanoporosity. Here we have examined km/s laser-driven flyer plate impacts on a prototypical MOF, ZIF-8. We observed particle fragmentation and morphological changes in microcrystals of ZIF-8 at lower shock pressures (≈2.5 GPa), and amorphization and structural col ...
DOI:
10.1021/jacs.6b12956

15. Small-Molecule Acceptor Based on the Heptacyclic Benzodi(cyclopentadithiophene) Unit for Highly Efficient Nonfullerene Organic Solar Cells

Author:
Kan Bin; Feng Huanran; Wan Xiangjian; Liu Feng; Ke Xin; Wang Yanbo; Wang Yunchuang; Zhang Hongtao; Li Chenxi; Hou Jianhui; Chen Yongsheng
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4929-4934
ISSN:
1520-5126
Subject:
absorption; energy; irradiation; photovoltaic cells; polymers; thermal stability
Abstract:
... A new nonfullerene small molecule with acceptor–donor–acceptor (A–D–A) structure, namely, NFBDT, based on a heptacyclic benzodi(cyclopentadithiophene) (FBDT) unit using benzo[1,2-b:4,5-b′]dithiophene as the core unit, was designed and synthesized. Its absorption ability, energy levels, thermal stability, as well as photovoltaic performances were fully investigated. NFBDT exhibits a low optical ban ...
DOI:
10.1021/jacs.7b01170

16. Stereochemistry of Endogenous Palmitic Acid Ester of 9-Hydroxystearic Acid and Relevance of Absolute Configuration to Regulation

Author:
Nelson Andrew T.; Kolar Matthew J.; Chu Qian; Syed Ismail; Kahn Barbara B.; Saghatelian Alan; Siegel Dionicio
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4943-4947
ISSN:
1520-5126
Subject:
adipose tissue; anti-inflammatory activity; biosynthesis; carboxylic ester hydrolases; enantiomers; fatty acid esters; hydroxy fatty acids; liquid chromatography; mass spectrometry; mice; palmitic acid; stereochemistry; transgenic animals
Abstract:
... Lipids have fundamental roles in the structure, energetics, and signaling of cells and organisms. The recent discovery of fatty acid esters of hydroxy fatty acids (FAHFAs), lipids with potent antidiabetic and anti-inflammatory activities, indicates that our understanding of the composition of lipidome and the function of lipids is incomplete. The ability to synthesize and test FAHFAs was critical ...
DOI:
10.1021/jacs.7b01269
PubMed:
28350171
PubMed Central:
PMC5568760

17. 4n–1 Is a “Sweet Spot” in DNA i-Motif Folding of 2′-Deoxycytidine Homopolymers

Author:
Fleming Aaron M.; Ding Yun; Rogers R. Aaron; Zhu Judy; Zhu Julia; Burton Ashlee D.; Carlisle Connor B.; Burrows Cynthia J.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4682-4689
ISSN:
1520-5126
Subject:
humans; models; nanotechnology; nucleotides; thymidine; pH; intergenic DNA; polymers; introns
Abstract:
... Strands of DNA with four or more contiguous runs of 2′-deoxycytidine (dC) nucleotides have the potential to adopt i-motif folds, generally under mildly acidic conditions. Analysis of dC homo-oligonucleotide strands ranging in length from 10 to 30 nucleotides by five different pH-dependent methods identified a pattern in strand length vs stability. Beginning with dC₁₁, which does not fold, the tran ...
DOI:
10.1021/jacs.6b10117

18. A General Strategy for Visible-Light Decaging Based on the Quinone Trimethyl Lock

Author:
Walton David P.; Dougherty Dennis A.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4655-4658
ISSN:
1520-5126
Subject:
absorption; amines; byproducts; hydroquinone; models
Abstract:
... Visible-light triggered quinone trimethyl locks are reported as a general design for long-wavelength photoremovable protecting groups for alcohols and amines. Intramolecular photoreduction unmasks a reactive phenol that undergoes fast lactonization to release alcohols and amines. Model substrates are released in quantitative yield along with well-defined, colorless hydroquinone byproducts. Substit ...
DOI:
10.1021/jacs.7b01548

19. A Metallo-molecular Cage That Can Close the Apertures with Coordination Bonds

Author:
Akine Shigehisa; Miyashita Masato; Nabeshima Tatsuya
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4631-4634
ISSN:
1520-5126
Subject:
chemical bonding; ligands
Abstract:
... We designed a novel tricobalt(III) metallo-molecular cage in which its apertures can be closed with bifunctional ligands via coordination bonds. A closed-cage complex was easily formed by ligand exchange of its open-cage analogue. Guest uptake/release by the open-cage complex was sufficiently fast to quickly reach guest-binding equilibrium, while that by the closed-cage complex was extremely slow ...
DOI:
10.1021/jacs.7b00840

20. A Study of the Mechanism of the Hydrogen Evolution Reaction on Nickel by Surface Interrogation Scanning Electrochemical Microscopy

Author:
Liang Zhenxing; Ahn Hyun S.; Bard Allen J.
Source:
Journal of the American Chemical Society 2017 v.139 no.13 pp. 4854-4858
ISSN:
1520-5126
Subject:
adsorption; electrochemistry; hydrogen; hydrogen production; microscopy; nickel
Abstract:
... The hydrogen evolution reaction (HER) on Ni in alkaline media was investigated by scanning electrochemical microscopy under two operating modes. First, the substrate generation/tip collection mode was employed to extract the “true” cathodic current associated with the HER from the total current in the polarization curve. Compared to metallic Ni, the electrocatalytic activity of the HER is improved ...
DOI:
10.1021/jacs.7b00279