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Dr. Sudipta Roy Christian J. Schürmann Totan Mondal Dr. Debasis Koley Dr. Regine Herbst‐Irmer Prof. Dr. Dietmar Stalke Prof. Dr. Herbert W. Roesky 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(36):12629-12633
Platinum dichalcogenides have been known to exhibit two‐dimensional layered structures. Herein, we describe the syntheses, isolation, and characterization of air‐stable crystalline cyclic alkyl(amino) carbene (cAAC)‐supported monomeric platinum disulfide three‐membered ring complex [(cAAC)2Pt(S2)] ( 2 ). The highly reactive platinum(0) [(cAAC)2Pt] complex ( 1 ) with two‐coordinate platinum activates elemental sulfur to give 2 . The brown crystals of bis‐carbene platinum(II)monosulfate [(cAAC)2Pt(SO4)x(S2)1?x] ( 4 ) have been isolated when the reaction was performed in air. The dioxygen analogue of 2 was formed upon exposing the THF solution of 1 to aerial oxygen (O2). The binding of oxygen at the Pt0 center was found to be reversible. Additionally, DFT study has been performed to elucidate the electronic structure and bonding scenario of 2 , 3 , and 4 . Quantum chemical calculations showed donor–acceptor‐type interaction for the Pt?S bonds in 2 and Pt?O bonds in 3 and 4 . 相似文献
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Direct Structural Identification of Gas Induced Gate‐Opening Coupled with Commensurate Adsorption in a Microporous Metal–Organic Framework
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Dr. Debasis Banerjee Hao Wang Dr. Anna M. Plonka Dr. Thomas J. Emge Dr. John B. Parise Prof. Dr. Jing Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(33):11816-11825
Gate‐opening is a unique and interesting phenomenon commonly observed in flexible porous frameworks, where the pore characteristics and/or crystal structures change in response to external stimuli such as adding or removing guest molecules. For gate‐opening that is induced by gas adsorption, the pore‐opening pressure often varies for different adsorbate molecules and, thus, can be applied to selectively separate a gas mixture. The detailed understanding of this phenomenon is of fundamental importance to the design of industrially applicable gas‐selective sorbents, which remains under investigated due to the lack of direct structural evidence for such systems. We report a mechanistic study of gas‐induced gate‐opening process of a microporous metal–organic framework, [Mn(ina)2] (ina=isonicotinate) associated with commensurate adsorption, by a combination of several analytical techniques including single crystal X‐ray diffraction, in situ powder X‐ray diffraction coupled with differential scanning calorimetry (XRD‐DSC), and gas adsorption–desorption methods. Our study reveals that the pronounced and reversible gate opening/closing phenomena observed in [Mn(ina)2] are coupled with a structural transition that involves rotation of the organic linker molecules as a result of interaction of the framework with adsorbed gas molecules including carbon dioxide and propane. The onset pressure to open the gate correlates with the extent of such interaction. 相似文献
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Rohit Kumar Dr. Sayan Dutta Vishal Sharma Praval P. Singh Dr. Rajesh G. Gonnade Prof. Debasis Koley Dr. Sakya S. Sen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(56):e202201896
In this work, two monomeric magnesium alkyl complexes ( 1 and 2 ) were prepared using bis(phosphino)carbazole framework and among them 1 has been used as a catalyst for hydroboration of alkenes and alkynes with pinacolborane (HBpin). A broad variety of aromatic and aliphatic alkenes and alkynes were efficiently reduced. Anti-Markovnikov regioselective hydroboration of alkenes and alkynes was achieved, which was confirmed by deuterium-labelling experiments. The work represents the first example of the use of magnesium in homogeneous catalytic hydroboration of alkene with broad substrate scope. Experimental mechanistic investigations and DFT calculations provided insights into the reaction mechanism. Finally, the hydroboration protocol was extended to terpenes. 相似文献
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Prof. Dr. Debasis Koley Sriman De Nardana Sivendran Prof. Dr. Lukas J. Gooßen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(61):15227-15239
In a combined experimental and computational study, the isomerization activity of the dinuclear palladium(I) complex [PdI(μ-Br)(PtBu3)]2 towards allyl arenes, esters, amides, ethers, and alcohols has been investigated. The calculated energy profiles for catalyst activation for two alternative dinuclear and mononuclear catalytic cycles, and for catalyst deactivation are in good agreement with the experimental results. Comparison of experimentally observed E/Z ratios at incomplete conversion with calculated kinetic selectivities revealed that a substantial amount of product must form via the dinuclear pathway, in which the isomerization is promoted cooperatively by two palladium centers. The dissociation barrier towards mononuclear Pd species is relatively high, and once the catalyst enters the energetically more favorable mononuclear pathway, only a low barrier has to be overcome towards irreversible deactivation. 相似文献
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