scholarly journals Manganese-Catalyzed Ammonia Oxidation into Dinitrogen

2020 ◽  
Author(s):  
Hiroki Toda ◽  
Kazunari Nakajima ◽  
Ken Sakata ◽  
Yoshiaki Nishibayashi
Keyword(s):  
Density Functional Theory ◽  
Dft Calculations ◽  
Density Functional ◽  
Ammonia Oxidation ◽  
Nucleophilic Attack ◽  
Mechanistic Studies ◽  
Oxidative Conversion ◽  
Functional Theory ◽  
Metal Catalyzed ◽  
Nitrogen Bond

Base metal-catalyzed oxidative conversion of ammonia into dinitrogen is a promising process to utilize ammonia as an energy carrier. In this study, we report the manganese-catalyzed ammonia oxidation under chemical and electrochemical conditions. Mechanistic studies including density functional theory (DFT) calculations suggest that a nucleophilic attack of ammonia on manganese nitrogenous complexes occurs to form a nitrogen–nitrogen bond leading to dinitrogen.<br>

scholarly journals Manganese-Catalyzed Ammonia Oxidation into Dinitrogen

2020 ◽  
Author(s):  
Hiroki Toda ◽  
Kazunari Nakajima ◽  
Ken Sakata ◽  
Yoshiaki Nishibayashi
Keyword(s):  
Density Functional Theory ◽  
Dft Calculations ◽  
Density Functional ◽  
Ammonia Oxidation ◽  
Nucleophilic Attack ◽  
Mechanistic Studies ◽  
Oxidative Conversion ◽  
Functional Theory ◽  
Metal Catalyzed ◽  
Nitrogen Bond

Base metal-catalyzed oxidative conversion of ammonia into dinitrogen is a promising process to utilize ammonia as an energy carrier. In this study, we report the manganese-catalyzed ammonia oxidation under chemical and electrochemical conditions. Mechanistic studies including density functional theory (DFT) calculations suggest that a nucleophilic attack of ammonia on manganese nitrogenous complexes occurs to form a nitrogen–nitrogen bond leading to dinitrogen.<br>

Development of transition-metal-catalyzed cycloaddition reactions leading to polycarbocyclic systems

2011 ◽  
Vol 83 (3) ◽  
pp. 495-506 ◽  
Author(s):  
Moisés Gulías ◽  
Fernando López ◽  
José L. Mascareñas
Keyword(s):  
Density Functional Theory ◽  
Transition Metal ◽  
Dft Calculations ◽  
Density Functional ◽  
Conjugated Dienes ◽  
Ni Catalysts ◽  
Functional Theory ◽  
Different Types ◽  
Transition Metal Catalyzed ◽  
Metal Catalyzed

We present a compilation of methodologies developed in our laboratories to assemble polycyclic structures containing small- and medium-sized cycles, relying on the use of transition-metal-catalyzed (TMC) cycloadditions. First, we discuss the use of alkylidenecyclopropanes (ACPs) as 3C-atom partners, in particular in their Pd-catalyzed (3 + 2) cycloadditions with alkynes, alkenes, and allenes, reactions that lead to cyclopentane-containing polycyclic products in excellent yields. Then, we present the expansion of this chemistry to a (4 + 3) annulation with conjugated dienes, and to inter- and intramolecular (3 + 2 + 2) cycloadditions using external alkenes as additional 2C-π-systems. These reactions allow the preparation of different types of polycyclic structures containing cycloheptene rings, the topology of the products depending on the use of Pd or Ni catalysts. Finally, we include our more recent discoveries on the development of (4 + 3) and (4 + 2) intramolecular cyclo-additions of allenes and dienes, promoted by Pt and Au catalysts, and discuss mechanistic insights supported by experimental and density functional theory (DFT) calculations. An enantioselective version of the (4 + 2) cycloaddition with phosphoramidite Au(I) catalysts is also presented.

scholarly journals Influence of Copper(I) Halides on the Reactivity of Aliphatic Carbodiimides

2020 ◽  
Vol 3 (1) ◽  
pp. 20
Author(s):  
Valentina Ferraro ◽  
Marco Bortoluzzi
Keyword(s):  
Density Functional Theory ◽  
Electronic Structure ◽  
General Formula ◽  
Electron Density ◽  
Density Functional ◽  
Functional Theory ◽  
Fukui Functions ◽  
Bond Lengths ◽  
Linear Complexes ◽  
Nitrogen Bond

The influence of copper(I) halides CuX (X = Cl, Br, I) on the electronic structure of N,N′-diisopropylcarbodiimide (DICDI) and N,N′-dicyclohexylcarbodiimide (DCC) was investigated by means of computational DFT (density functional theory) methods. The coordination of the considered carbodiimides occurs by one of the nitrogen atoms, with the formation of linear complexes having a general formula of [CuX(carbodiimide)]. Besides varying the carbon–nitrogen bond lengths, the thermodynamically favourable interaction with Cu(I) reduces the electron density on the carbodiimides and alters the energies of the (NCN)-centred, unoccupied orbitals. A small dependence of these effects on the choice of the halide was observable. The computed Fukui functions suggested negligible interaction of Cu(I) with incoming nucleophiles, and the reactivity of carbodiimides was altered by coordination mainly because of the increased electrophilicity of the {NCN} fragments.

γ-Valerolactone-Introduced Controlled-Isomerization of Glucose for Lactic Acid Production over Sn-Beta Catalyst

2021 ◽  
Author(s):  
Xinpeng Zhao ◽  
Zhimin Zhou ◽  
hu luo ◽  
Yanfei Zhang ◽  
Wang Liu ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Lactic Acid ◽  
Dft Calculations ◽  
Acid Production ◽  
Density Functional ◽  
Lactic Acid Production ◽  
Hydrothermal Conversion ◽  
Functional Theory ◽  
Environment Friendly

Combined experiments and density functional theory (DFT) calculations provided insights into the role of the environment-friendly γ-valerolactone (GVL) as a solvent in the hydrothermal conversion of glucose into lactic acid...

Mechanistic understanding of the Cu(i)-catalyzed domino reaction constructing 1-aryl-1,2,3-triazole from electron-rich aryl bromide, alkyne, and sodium azide: a DFT study

2021 ◽  
Author(s):  
Hanlin Gan ◽  
Liang Peng ◽  
Feng Long Gu
Keyword(s):  
Density Functional Theory ◽  
Dft Calculations ◽  
Sodium Azide ◽  
Density Functional ◽  
Dft Study ◽  
Domino Reaction ◽  
Aryl Bromide ◽  
Functional Theory ◽  
Mechanistic Understanding

The mechanism of the Cu(i)-catalyzed domino reaction furnishing 1-aryl-1,2,3-triazole assisted by CuI and 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) is explored with density functional theory (DFT) calculations.

scholarly journals Density functional theory (DFT) calculations of VI/V reduction potentials of uranyl coordination complexes in non-aqueous solutions

2019 ◽  
Vol 21 (6) ◽  
pp. 3227-3241 ◽  
Author(s):  
Krishnamoorthy Arumugam ◽  
Neil A. Burton
Keyword(s):  
Density Functional Theory ◽  
Dft Calculations ◽  
Aqueous Solutions ◽  
Density Functional ◽  
Coordination Complexes ◽  
Dft Study ◽  
Redox Behavior ◽  
Functional Theory ◽  
Reduction Potentials ◽  
Uranium Complexes

Of particular interest within the +6 uranium complexes is the linear uranyl(vi) cation and it forms numerous coordination complexes in solution and exhibits incongruent redox behavior depending on coordinating ligands. This DFT study predicts VI/V reduction potentials of a range of uranyl(vi) complexes in non-aqueous solutions within ∼0.10−0.20 eV of experiment.

scholarly journals Iron(II) complexes of dimethyltriazacyclophane

2018 ◽  
Vol 74 (12) ◽  
pp. 1641-1649
Author(s):  
Wei-Tsung Lee ◽  
Matthias Zeller ◽  
David Upp ◽  
Yuliya Politanska ◽  
Doug Steinman ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Solid State ◽  
Dft Calculations ◽  
Density Functional Calculations ◽  
Density Functional ◽  
Coordination Mode ◽  
Functional Theory ◽  
Metal Centers ◽  
Bonding Interaction

Treatment of the ortho-triazacyclophane 1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-triene [(C6H5)3(NH)(NCH3)2, L1] with Fe[N(SiMe3)2]2 yields the dimeric iron(II) complex bis(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido)bis[(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido)iron(II)], [Fe(C20H18N3)4] or Fe2(L1)4 (9). Dissolution of 9 in tetrahydrofuran (THF) results in solvation by two THF ligands and the formation of a simpler monoiron complex, namely bis(μ-1,4-dimethyltribenzo[b,e,h][1,4,7]triazacyclonona-2,5,8-trien-7-ido-κN 7)bis(tetrahydrofuran-κO)iron(II), [Fe(C20H18N3)2(C4H8O)2] or (L1)2Fe(THF)2 (10). The reaction is reversible and 10 reverts in vacuo to diiron complex 9. In the structures of both 9 and 10, the monoanionic triazacyclophane ligand L1− is observed in only the less-symmetric saddle conformation. No bowl-shaped crown conformers are observed in the solid state, thus preventing chelating κ3-coordination to the metal as had been proposed earlier based on density functional theory (DFT) calculations. Instead, the L1− ligands are bound in either a η2-chelating fashion through the amide and one amine donor (for one of the four ligands of 9), or solely through their amide N atoms in an even simpler monodentate η1-coordination mode. Density functional calculations on dimer 9 revealed nearly full cationic charges on each Fe atom and no bonding interaction between the two metal centers, consistent with the relatively long Fe...Fe distance of 2.912 (1) Å observed in the solid state.

Synthesis, characterization, crystal structure and density functional theory (DFT) calculations of dioxomolybdenum (VI) complexes of an ONS donor ligand derived from benzoylacetone and S-benzyl dithiocarbazate

Polyhedron ◽  
2013 ◽  
Vol 50 (1) ◽  
pp. 602-611 ◽  
Author(s):  
Manashi Chakraborty ◽  
Sathi Roychowdhury ◽  
Nikhil Ranjan Pramanik ◽  
Tapas Kumar Raychaudhuri ◽  
Tapan Kumar Mondal ◽  
...  
Keyword(s):  
Crystal Structure ◽  
Density Functional Theory ◽  
Dft Calculations ◽  
Density Functional ◽  
Functional Theory ◽  
Donor Ligand

The Pivotal Alkyne Group in the Mutual Size-Conversion of Au9 with Au10 Nanoclusters

2021 ◽  
Author(s):  
Xiaohang Wu ◽  
Ying Lv ◽  
Yuyuan Bai ◽  
Haizhu Yu ◽  
Manzhou Zhu
Keyword(s):  
Density Functional Theory ◽  
Theoretical Model ◽  
Dft Calculations ◽  
Density Functional ◽  
Single Atom ◽  
Functional Theory

Herein, density functional theory (DFT) calculations were performed to elucidate the mechanism of the reversible single atom size conversion between [Au10(DMPP)4(C6H11C≡C)]3+ and [Au9(DMPP)4]3+ (DMPP is 2,2’-bis-(dimethylphosphino)-1,1’-biphenyl, the simplified, theoretical model...

Design and Prediction of High Potent ansa-Zirconocene for Olefin Polymerizations: Combined DFT Calculations and QSPR Approach

2021 ◽  
Author(s):  
Manussada Ratanasak ◽  
Jun-ya Hasegawa ◽  
Vudhichai Parasuk
Keyword(s):  
Density Functional Theory ◽  
Dft Calculations ◽  
Density Functional ◽  
Functional Theory ◽  
Olefin Polymerizations

Homopolymerization of ethene (ET), propene (PP), 1-butene (BT), 1-hexene (HX), and styrene (ST) by rac [Zr{1-Me2Si(3-Pr-(η5-C9H5))(3-H-(η5-C9H5))Cl2] ansa-zirconocene catalyst were investigated using Density Functional Theory (DFT) calculations. This study unveiled the...

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