14 Nov 18:38
by Hyoyoung Lee,
Thi Anh Le,
Ngoc Quang Tran,
Yeseul Hong
Electrode architecture: Intertwined titanium carbide MXene within a tangled polypyrrole nanowire matrix is prepared and demonstrated as a novel hybridization electrode with outstanding gravimetric capacitance (610 F g−1) and stability (14 000 cycles) compared with reported MXene‐based supercapacitors (see figure).
Abstract
The exploration of the rational design and synthesis of unique and robust architectured electrodes for the high capacitance, rate capability, and stability of supercapacitors is crucial to the future of energy storage technology. Herein, an in situ synthesis of multilayered titanium carbide MXene tightly caging within a 3 D conducting tangled polypyrrole (PPy) nanowire (NW) network is proposed as an effective strategy to prevent the aggregation of MXene, profoundly enhancing the electrochemical performance of the supercapacitor. Owing to the beneficial effects of an ideal 3 D interconnected porous structure and high electrical conductivity, the obtained electrode exhibits fast charge and ion transport kinetics as well as full usage of active material. As expected, the 3 D Ti3C2T
x
@PPY NW exhibits a specific capacitance five times higher than that of pristine MXene (610 F g−1), a good rate capability up to a current density of 25 A g−1, and excellent stability with 100 % retention after 14 000 cycles at 4 A g−1, outperforming the known state‐of‐the‐art MXene‐based supercapacitor. Our work provides a facile method for enhancing the performance of MXene‐based energy storage devices.
26 Apr 21:23
by Proctor, R. S. J., Davis, H. J., Phipps, R. J.
Basic heteroarenes are a ubiquitous feature of pharmaceuticals and bioactive molecules, and Minisci-type additions of radical nucleophiles are a leading method for their elaboration. Despite many Minisci-type protocols that result in the formation of stereocenters, exerting control over the absolute stereochemistry at these centers remains an unmet challenge. We report a process for addition of prochiral radicals, generated from amino acid derivatives, to pyridines and quinolines. Our method offers excellent control of both enantioselectivity and regioselectivity. An enantiopure chiral Brønsted acid catalyst serves both to activate the substrate and induce asymmetry, while an iridium photocatalyst mediates the required electron transfer processes. We anticipate that this method will expedite access to enantioenriched small-molecule building blocks bearing versatile basic heterocycles.
19 Mar 12:05
by Kaila A. Margrey, William L. Czaplyski, David A. Nicewicz and Erik J. Alexanian

Journal of the American Chemical Society
DOI: 10.1021/jacs.8b00592
28 Jun 05:27
by Jeppe Kari, Morten Andersen, Kim Borch and Peter Westh

ACS Catalysis
DOI: 10.1021/acscatal.7b00838
31 Oct 00:31
by Mingbing Zhong, Song Sun, Jiang Cheng and Ying Shao

The Journal of Organic Chemistry
DOI: 10.1021/acs.joc.6b01910
30 Sep 20:59
by Rodolphe Beaud, Robert J. Phipps and Matthew J. Gaunt

Journal of the American Chemical Society
DOI: 10.1021/jacs.6b09334
大河真弯, XJ and 8 others like this
17 May 00:21
by Susan L. Zultanski, Jingyi Zhao and Shannon S. Stahl

Journal of the American Chemical Society
DOI: 10.1021/jacs.6b03931
26 Feb 03:52
by Simon J. Freakley
The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 represents a potentially atom-efficient alternative to the current industrial indirect process. We show that the addition of tin to palladium catalysts coupled with an appropriate heat treatment cycle switches off the sequential hydrogenation and decomposition reactions, enabling selectivities of >95% toward H2O2. This effect arises from a tin oxide surface layer that encapsulates small Pd-rich particles while leaving larger Pd-Sn alloy particles exposed. We show that this effect is a general feature for oxide-supported Pd catalysts containing an appropriate second metal oxide component, and we set out the design principles for producing high-selectivity Pd-based catalysts for direct H2O2 production that do not contain gold.
Authors: Simon J. Freakley, Qian He, Jonathan H. Harrhy, Li Lu, David A. Crole, David J. Morgan, Edwin N. Ntainjua, Jennifer K. Edwards, Albert F. Carley, Albina Y. Borisevich, Christopher J. Kiely, Graham J. Hutchings
19 Apr 02:11
by Nerea Conde, Fátima Churruca, Raul SanMartin, María Teresa Herrero, Esther Domínguez
Abstract
The direct arylation of N-substituted o-bromobenzanilides and benzenesulfonamides via C
H bond functionalization has been developed using very low catalyst loadings. This novel cost-effective and more sustainable method relies on a PCN-type palladium pincer complex as a highly active palladium source, providing a general and efficient access to phenanthridinones, biaryl sultams and related heterocyclic systems. The beneficial effect of water as cosolvent has been observed in this process, which is not seriously influenced by electronic effects at the arene moieties or sterically demanding substituents at the amide or sulfonamide nitrogen. In addition, a number of experiments (kinetic plot, poisoning assays, TEM, ESI) have been performed in order to understand the role of the employed palladium complex in this reaction.
22 Jan 05:58
by Songjie Yu, Song Liu, Yu Lan, Boshun Wan and Xingwei Li

Journal of the American Chemical Society
DOI: 10.1021/ja511796h
04 Nov 03:33
by Sylvia Flaig, Johanna Akbarzadeh, Paolo Dolcet, Silvia Gross, Herwig Peterlik, Nicola Hüsing
Abstract
Hierarchically organized silica–titania monoliths were synthesized under purely aqueous conditions by applying a new ethylene glycol-modified single-source precursor, such as 3-[3-{tris(2-hydroxyethoxy)silyl}propyl]acetylacetone coordinated to a titanium center. The influence of the silicon- and titanium-containing single-source precursor, the novel glycolated organofunctional silane, and the addition of tetrakis(2-hydroxyethyl)orthosilicate on the formation of the final porous network was investigated by SEM, TEM, nitrogen sorption, and SAXS/WAXS. In situ SAXS measurements were performed to obtain insight into the development of the mesoporous network during sol–gel transition. IR-ATR, UV/Vis, XPS, and XAFS measurements showed that up to a Si/Ti ratio of 35:1, well-dispersed titanium centers in a macro-/mesoporous SiO2 network with a specific surface area of up to 582 m2 g−1 were obtained. An increase in Ti content resulted in a decrease in specific surface area and a loss of the cellular character of the macroporous network. With a 1:1 Si/Ti ratio, silica–titania powders with circa 100 m2 g−1 and anatase domains within the SiO2 matrix were obtained.
Hierarchically organized SiO2/TiO2 monoliths were synthesized in purely aqueous conditions by applying an ethylene glycol modified single-source precursor (SSP), such as 3-[3-{tris(2-hydroxyethoxy)silyl}propyl]acetylacetonate coordinated to a titanium center. The influence of the SSP on the formation of the final porous network was investigated. The homogeneity of the Si and Ti centers in the oxide matrix was also investigated.
27 Apr 00:11
by B. T. Worrell
The mechanism of a common and highly versatile molecular coupling reaction is elucidated.
Authors: B. T. Worrell, J. A. Malik, V. V. Fokin
19 Apr 02:29
by Olga Lifchits, Manuel Mahlau, Corinna M. Reisinger, Anna Lee, Christophe Farès, Iakov Polyak, Gopinadhanpillai Gopakumar, Walter Thiel and Benjamin List

Journal of the American Chemical Society DOI: 10.1021/ja402058v