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Synthesis of Lewis acid-base adducts between potassium dihydrogenpnictogenides and group 13 Lewis acids.
Chemistry
December 2024
Philipps-Universität Marburg: Philipps-Universitat Marburg, Department of Chemistry, Hans-Meerwein-Straße 4, 35032, Marburg, GERMANY.
Lewis acid-base adducts between potassium dihydrogenpnictogenides [K(18c6)PnH2] (Pn = P, As) and Trialkylgallanes (GaMe3, GaEt3, GatBu3) as well as BH3 were synthesized. In the course of these investigations, we were able to fully characterize a row of compounds of the type [K(18c6)(thf)0‑2][PnH2(ER3)2] (E = B: R = H; E = Ga: R = Me, Et, tBu). Based on the successful syntheses of these species, we also synthesized several compounds of the composition [K(18c6)(thf)0‑2][Pn(SiMe3)2(ER3)n] (n = 1, 2) starting from [KPn(SiMe3)2] (Pn = P and As) and ER3 (E = B, Al, In: R = Me; E = Ga: R= Me, Et, tBu).
View Article and Find Full Text PDFComputational Study of Electrochemical CO Reduction on 2D Graphitic Carbon Nitride Supported Single-Atom (Al and P) Catalysts (SACs).
Chemphyschem
December 2024
Department of Nanoscience, Joint School of Nanoscience & Nanoengineering (JSNN), University of North Carolina at Greensboro, Greensboro, NC 27401, USA.
To mitigate the adverse effects of CO emissions, CO electroreduction to small organic products is a preferable solution and potential catalysts include the single-atom catalyst (SAC) which comprises individual atoms dispersed on 2D materials. Here, we used aluminum and phosphorus as the active sites for CO electroreductions by embedding them on the 2D graphitic carbon nitride (g-CN) nano-surface. The resulting M-CN (M=Al and P) SACs were computationally studied for the CO electroreduction using density functional theory (DFT) and ab-initio molecular dynamics (AIMD) simulations.
View Article and Find Full Text PDFExamining the reactivity of oxygen-bridged intramolecular group 13 element/phosphorus and boron/group 15 element frustrated Lewis pairs in 1,2-addition reactions with CS.
Phys Chem Chem Phys
December 2024
Department of Applied Chemistry, National Chiayi University, Chiayi 60004, Taiwan.
The 1,2-addition reactions involving CS and oxygen-bridged intramolecular G13/P-based (G13 = group 13 element) and B/G15-based (G15 = group 15 element) frustrated Lewis pairs (FLPs) have been theoretically analyzed through density functional theory (DFT). Our DFT calculations suggest that of the nine FLP-assisted compounds, only B/P-Rea, Al/P-Rea, Ga/P-Rea, and In/P-Rea can kinetically and thermodynamically initiate energetically favorable 1,2-addition reactions with CS, forming five-membered heterocyclic adducts. Our findings from the activation strain model suggest that the atomic radius of the Lewis acceptor (G13) and donor (G15) is critical in setting the barrier heights needed for optimal orbital interactions between G13/P-Rea, B/G15-Rea, and CS.
View Article and Find Full Text PDFZwitterionic 2-Phosphaethene-thiolates [(L)P=CS(L)] as PCS Building Blocks (L=NHC, L=PR).
Angew Chem Int Ed Engl
November 2024
Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01062, Dresden, Germany.
Article Synopsis
- The zwitterionic compounds [(L)P=CS(L)] (3), synthesized as triflate salts, show promise as building blocks for PCS (phosphorus-containing species) by reacting with various electrophiles and nucleophiles for selective functionalization.
- These compounds can act as ambident nucleophiles and create a unique linear coordination polymer with AgOTf, marking a significant step in transition metal complex applications.
- Reduction of 3 leads to the formation of the [PCS] anion, while cycloaddition reactions create polyphosphorus heterocycles, indicating potential for further exploration of the C-S bond activation in future research.
Oxaphosphiranes: isolable phosphorus-containing epoxide rings.
Dalton Trans
December 2024
Institut für Anorganische Chemie, der Rheinischen Friedrich-Wilhelms-Universität Bonn, Gerhard-Domagk-Str. 1, 53121, Bonn, Germany.
Combining different heteroatoms in an epoxide-type ring having Lewis basic and acidic characteristics is challenging as it creates an increasing number of polar bonds and high ring strain energy. The first examples of isolable oxaphosphiranes, , epoxide rings with a phosphorus atom, have been synthesized using a facile and effective protocol starting from [pentacarbonyl{dichloro(trityl)phosphane}molybdenum(0)] (trityl = CPh), -butyllithium and commercially available fluorinated benzaldehydes. Reactions with various acids and bases will be described.
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