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08 Oct 07:12

[ASAP] High Turnover Pd/C Catalyst for Nitro Group Reductions in Water. One-Pot Sequences and Syntheses of Pharmaceutical Intermediates

by Xiaohan Li, Ruchita R. Thakore, Balaram S. Takale, Fabrice Gallou, and Bruce H. Lipshutz

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Organic Letters
DOI: 10.1021/acs.orglett.1c03258
07 Oct 09:41

Water Splitting by C60‐Supported Vanadium Single Atoms

by Gao-Lei Hou, Tao Yang, Meng-Yang Li, Jan Vanbuel, Olga V. Lushchikova, Piero Ferrari, Joost M. Bakker, Ewald Janssens
Water Splitting by C60-Supported Vanadium Single Atoms

Splitting of water by a single vanadium is greatly facilitated by a C60 support, which can be regarded as a small piece of porous carbon nanomaterials, especially those with intrinsic pentagonal defects and curvatures. The compelling experimental and theoretical evidence demonstrates the important role of support in single vanadium atom catalysis.


Abstract

Water splitting is an important source of hydrogen, a promising future carrier for clean and renewable energy. A detailed understanding of the mechanisms of water splitting, catalyzed by supported metal atoms or nanoparticles, is essential to improve the design of efficient catalysts. Here, we report an infrared spectroscopic study of such a water splitting process, assisted by a C60 supported vanadium atom, C60V++H2O→C60VO++H2. We probe both the entrance channel complex C60V+(H2O) and the end product C60VO+, and observe the formation of H2 as a result from resonant infrared absorption. Density functional theory calculations exploring the detailed reaction pathway reveal that a quintet-to-triplet spin crossing facilitates the water splitting reaction by C60-supported V+, whereas this reaction is kinetically hindered on the isolated V+ ion by a high energy barrier. The C60 support has an important role in lowering the reaction barrier with more than 70 kJ mol−1 due to a large orbital overlap of one water hydrogen atom with one carbon atom of the C60 support. This fundamental insight in the water splitting reaction by a C60-supported single vanadium atom showcases the importance of supports in single atom catalysts by modifying the reaction potential energy surface.

07 Oct 09:38

[ASAP] Catalytic Conversion of Lignin to Liquid Fuels with an Improved H/Ceff Value over Bimetallic NiMo-MOF-Derived Catalysts

by Changzhou Chen, Peng Liu, Haihong Xia, Jianchun Jiang, Xiaohui Yang, and Minghao Zhou

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ACS Sustainable Chemistry & Engineering
DOI: 10.1021/acssuschemeng.1c05273
28 Sep 14:57

Electrochemical Reductive Arylation of Nitroarenes with Arylboronic Acids

by Dan Wang, Zhaohua Wan, Heng Zhang, Hesham Alhumade, Hong Yi, Aiwen Lei
Electrochemical Reductive Arylation of Nitroarenes with Arylboronic Acids

Reductive arylation: The synthesis of diarylamine is extremely important in organic chemistry. Herein, a novel electrochemical reductive arylation of arylboronic acids with nitroarenes is developed. A variety of diarylamines is synthesized without the need for transition-metal catalysts. The reaction can be scaled up efficiently in a flow cell and several derivatization reactions are carried out smoothly.


Abstract

The synthesis of diarylamine is extremely important in organic chemistry. Herein, a novel electrochemical reductive arylation of nitroarenes with arylboronic acids was developed. A variety of diarylamines were synthesized without the need for transition-metal catalysts. The reaction could be scaled up efficiently in a flow cell and several derivatization reactions were carried out smoothly. Cyclic voltammetry experiments and mechanism studies showed that acetonitrile, formic acid, and triethyl phosphite all played a role in promoting this reductive arylation transformation.

24 Sep 08:20

[ASAP] Cu-Catalyzed Cross-Coupling of Nitroarenes with Aryl Boronic Acids to Construct Diarylamines

by Xinyu Guan, Haoran Zhu, and Tom G. Driver

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ACS Catalysis
DOI: 10.1021/acscatal.1c03113
23 Sep 09:36

Sustainable production of pharmaceutical, nutraceutical and bioactive compounds from biomass and waste

Mathias

Can anybody fix a PDF?

Chem. Soc. Rev., 2021, 50,11191-11207
DOI: 10.1039/D1CS00524C, Tutorial Review
Claudia Espro, Emilia Paone, Francesco Mauriello, Roberto Gotti, Elisa Uliassi, Maria Laura Bolognesi, Daily Rodríguez-Padrón, Rafael Luque
The aim of this tutorial review is to provide a general overview of processes, technologies and challenges in the production of pharmaceutical and bioactive compounds from food waste and lignocellulosic residues.
The content of this RSS Feed (c) The Royal Society of Chemistry
16 Sep 15:02

[ASAP] Oxidative Catalytic Fractionation of Lignocellulosic Biomass under Non-alkaline Conditions

by Hao Luo, Eric P. Weeda, Manar Alherech, Colin W. Anson, Steven D. Karlen, Yanbin Cui, Cliff E. Foster, and Shannon S. Stahl

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Journal of the American Chemical Society
DOI: 10.1021/jacs.1c08635
10 Sep 15:21

Hydrothermal Degradation of Amino Acids

by Paul Körner
Mathias

@CVE @LM

Hydrothermal Degradation of Amino Acids

The missing part: It is well known that hydrothermal processes can be used to convert biomass into solid, liquid, or even gaseous fuels. There are also innumerable scientific reports about the degradation of carbohydrates under hydrothermal conditions yielding especially furanic compounds. Fatty acids, in turn, can be expected to be rather inert during hydrothermal treatment. But what happens to another integral component of biomass: amino acids?


Abstract

Within the past years, hydrothermal processes have gathered much attention as promising conversion technologies for especially wet biomass. Amino acids are an integral component of biomass, zoo biomass in particular. However, what happens to them during hydrothermal treatment? Reviewing the available literature going back to the mid of the 20th century revealed an astonishing, but still fragmentary view. In fact, two universal degradation reactions could be identified (i. e., deamination and decarboxylation), competing with each other. Thereby, small structural differences may obviously have huge impacts on the fate of individual amino acids. Nevertheless, the amount of available experimental data is relatively scarce in many cases. In this work, the available knowledge about the degradation of 20 proteinogenic amino acids under hydrothermal conditions was presented and discussed critically. The hydrothermal conversion of proteinaceus biomass as well as the Maillard reaction, both extensively reviewed elsewhere, were only touched on.

08 Sep 12:34

Palladium‐Catalyzed Decarboxylative 1,2‐Addition of Carboxylic Acids to Glyoxylic Acid Esters

by Bastian Jakob, Ichraf Slimani, Andreas Diehl, Naceur Hamdi, Georg Manolikakes
Palladium-Catalyzed Decarboxylative 1,2-Addition of Carboxylic Acids to Glyoxylic Acid Esters

A Palladium-catalyzed 1,2-addition reaction of carboxylic acids to glyoxylic acid esters is reported. This method provides access to mandelic acid derivatives from simple, readily available starting materials in good yields. Carboxylic acids are utilized as more sustainable alternative to common organometallic nucleophiles.


Abstract

The formation of C−C-bonds constitutes one of the most fundamental synthetic operations in organic chemistry. The nucleophilic addition of preformed organometallic reagents to an electrophilic carbonyl functionality represents a classical method for the selective construction of a C−C-bond. However, the synthesis and utilization of an organometallic reagent is associated with an unfavorable environmental profile. Herein, we disclose a Palladium-catalyzed decarboxylative 1,2-addition of carboxylic acids to glyoxylic acid esters. This novel method provides access to the mandelic acid scaffold in good yields. Easy-to-handle and readily available benzoic acids are utilized as more sustainable alternative to preformed organometallic nucleophiles.

06 Sep 08:41

[ASAP] Photocatalytic Reductive C–O Bond Cleavage of Alkyl Aryl Ethers by Using Carbazole Catalysts with Cesium Carbonate

by Tatsushi Yabuta, Masahiko Hayashi, and Ryosuke Matsubara

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The Journal of Organic Chemistry
DOI: 10.1021/acs.joc.0c02663