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Room-Temperature Formate Ester Transfer Hydrogenation Enables an Electrochemical/Thermal Organometallic Cascade for Methanol Synthesis from CO.
Angew Chem Int Ed Engl
November 2024
Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States.
The reduction of CO to synthetic fuels is a valuable strategy for energy storage. However, the formation of energy-dense liquid fuels such as methanol remains rare, particularly under low-temperature and low-pressure conditions that can be coupled to renewable electricity sources via electrochemistry. Here, a multicatalyst system pairing an electrocatalyst with a thermal organometallic catalyst is introduced, which enables the reduction of CO to methanol at ambient temperature and pressure.
View Article and Find Full Text PDFIntegrated electrochemical CO reduction and hydroformylation.
Dalton Trans
December 2024
Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
The development of integrated multi-catalyst processes has become of high interest to transform abundant feedstocks or environmental pollutants to commodity chemicals in a one pot, one pass fashion. Specifically, CO poses a large environmental burden and would thus be a desirable, relatively abundant C1 source in multi-step synthetic chemistry. Herein we disclose the synthesis of aldehydes from CO the integration of electrochemical CO reduction (CORR) and hydroformylation, taking advantage of the typically unwanted concomitant hydrogen evolution (HER) to generate the necessary CO and H needed for hydroformylation.
View Article and Find Full Text PDFArtificial plant cell walls as multi-catalyst systems for enzymatic cooperative asymmetric catalysis in non-aqueous media.
Chem Commun (Camb)
September 2021
Department of Natural Sciences, Mid Sweden University, Holmgatan 10, 85 179 Sundsvall, Sweden.
The assembly of cellulose-based artificial plant cell wall (APCW) structures that contain different types of catalysts is a powerful strategy for the development of cascade reactions. Here we disclose an APCW catalytic system containing a lipase enzyme and nanopalladium particles that transform a racemic amine into the corresponding enantiomerically pure amide in high yield via a dynamic kinetic resolution.
View Article and Find Full Text PDFStepwise Electrocatalysis as a Strategy against Polysulfide Shuttling in Li-S Batteries.
ACS Nano
December 2019
Department of Chemical and Biomolecular Engineering , National University of Singapore, Singapore 119260 , Singapore.
Most issues with Li-S batteries are caused by the slowness of the multielectron sulfur electrochemical reaction resulting in the loss of sulfur as soluble polysulfides to the electrolyte and the redox shuttling of polysulfides between the cathode and anode during battery charge and discharge. The acceleration of the polysulfide conversion reaction to their end products electrocatalysis has the appeal of a root-cause solution. However, the polysulfide electrocatalysts developed to date have rarely considered polysulfide conversion as a multistep reaction and, as such, were not optimized to target specific steps in the overall S ↔ LiS ↔ LiS conversion.
View Article and Find Full Text PDFMerging Visible-Light Photoredox and Chiral Phosphate Catalysis for Asymmetric Friedel-Crafts Reaction with in Situ Generation of N-Acyl Imines.
Org Lett
May 2019
Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemistry , University of Science and Technology of China, Hefei 230026 , China.
In the presence of visible-light photoredox and chiral phosphate catalysts, a novel asymmetric Friedel-Crafts reaction of indoles and readily accessible α-amino acid derived redox-active esters is established to afford enantioenriched 1-indolyl-1-alkylamine derivatives in moderate to high yields and with high levels of enantioselectivities. This method not only shows a mild and efficient alternative for the in situ generation of N-acyl imines but also indicates the feasibility of a multicatalyst system for asymmetric photoredox catalysis.
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