Iron-Catalyzed Hydrogenation of Alkyl Formates and Carbon Dioxide

Organometallics, Год журнала: 2025, Номер unknown

Опубликована: Фев. 13, 2025

Язык: Английский

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Opportunities for the renewable energy transition via reactive carbon capture

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This viewpoint article gives a brief overview of reactive carbon capture (RCC) and its relationship to traditional (CC) technologies discusses possible roles for RCC in the transition renewable energy economy.

Язык: Английский

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Recent developments in first-row transition metal complex-catalyzed CO₂ hydrogenation

Dalton Transactions, Год журнала: 2022, Номер 51(21), С. 8160 - 8168

Опубликована: Янв. 1, 2022

First-row transition metal catalyzed CO 2 hydrogenation heralds a new dawn in managment technology.

Язык: Английский

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Combined Computational and Experimental Investigation on the Mechanism of CO₂ Hydrogenation to Methanol with Mn-PNP-Pincer Catalysts

ACS Catalysis, Год журнала: 2022, Номер 12(24), С. 15310 - 15322

Опубликована: Ноя. 30, 2022

A theoretical and experimental mechanistic study is presented for the homogeneously catalyzed CO2 hydrogenation to methanol, using an Mn-PNP-Pincer catalyst in presence of a Lewis acid cocatalyst alcohol as solvent. Quantum chemical computations at density functional theory DLPNO-CCSD(T) level suggest formate resting state most stable intermediate. The concerted activation dihydrogen via proton shuttle mechanism decomposition hemiacetal intermediate computed define turnover-determining transition state. resulting energy span calculated 34.5 kcal mol–1 theory. An Eyring plot reveals barrier reaction 31.4 under catalytic turnover conditions, showing good agreement with slight overestimation computational model. Concentration–time profiles involved species also locate experimentally rate-determining states (RDSs) ester methanol. measured kinetic isotope effects use H2/D2 EtOH/D are hydrogen splitting RDS, giving further support mechanism. These insights provide guidance reference future improvement catalysts based on abundant 3d metals CO2-based production

Язык: Английский

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Homogeneous Metal-Catalyzed Hydrogenation of CO2 Derivatives: Towards Indirect Conversion of CO2 to Methanol

Inorganics, Год журнала: 2023, Номер 11(7), С. 302 - 302

Опубликована: Июль 15, 2023

The increase in anthropogenic CO2 concentrations and associated environmental issues have demanded the development of technologies for utilization. Among various potential solutions to decrease emissions achieve carbon neutrality, recycling post-combustion into value-added chemicals fuels is considered one most economically attractive processes. In this regard, due its large global demand versatile applications chemical energy sectors, methanol serves as appealing target utilization CO2. However, direct hydrogenation MeOH has proved challenging selectivity high input, mainly dependent on CO2-emitting fossil sources. To address these challenges, an alternative indirect CO2-to-MeOH methodology been proposed, which involves via intermediate formation well-known derivatives, such formates, carbonates, formamides, carbamates, urea derivatives. Homogeneous transition metal catalysts at center research avenue, potentially allowing more selective low-temperature routes from MeOH. This review aims highlight advances challenges homogeneous metal-catalyzed major derivatives Special attention paid mechanisms transformations.

Язык: Английский

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Homogeneous Hydrogenation of CO₂ and CO to Methanol: The Renaissance of Low‐Temperature Catalysis in the Context of the Methanol Economy

Angewandte Chemie, Год журнала: 2022, Номер 134(42)

Опубликована: Авг. 3, 2022

Abstract The traditional economy based on carbon‐intensive fuels and materials has led to an exponential rise in anthropogenic CO 2 emissions. Outpacing the natural carbon cycle, atmospheric levels increased by 50 % since pre‐industrial age can be directly linked global warming. Being at core of proposed methanol pioneered late George A. Olah, chemical recycling produce methanol, a green fuel feedstock, is prime channel achieve neutrality. In this direction, homogeneous catalytic systems have lately been major focus for synthesis from , their derivatives as potential low‐temperature alternatives commercial processes. This Review provides account rapidly growing field over past decade, its resurgence 2011. Based critical assessment progress thus far, present key challenges highlighted directions suggested practically viable applications.

Язык: Английский

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Heteroleptic Palladium(II) Complexes of Thiazolinyl‐picolinamide Derived N^∩N^∩N Pincer Ligand: An Efficient Catalyst for Acylative Suzuki Coupling Reactions

Asian Journal of Organic Chemistry, Год журнала: 2021, Номер 10(11), С. 2982 - 2992

Опубликована: Сен. 22, 2021

Abstract Synthesis, reactivity, characterization, and catalytic activities of a series palladium(II) complexes containing the thiazolinyl‐picolinamide derived pincer ligand is reported. Treatment 2‐aminobenzonitrile with cysteamine subsequent treatment 2‐picolinic acid afforded tridentate N ∩ ( 2 ). either (COD)PdCl or PdCl in 1 : ratio complex [(κ 3 ‐N N)PdCl] A reaction between Pd(OAc) equimolar dichloromethane gave N)Pd(η ‐OAc)] 4 ) which on further triflic acetonitrile produced N)Pd(N≡C−CH )]OTf 5 The was treated auxiliary ligands to produce cationic heteroleptic palladium complexes, N)Pd(NC H 6 ), CN)]OTf 7 NMe 8 respectively. newly synthesized compounds were characterized by 13 C{ H} NMR spectroscopic techniques molecular structures – , established. activity evaluated for acylative Suzuki coupling aryl carboxylic acids arylboronic yield unsymmetrically substituted biaryl ketones. effect conditions viz ., solvent, base, temperature, catalyst loading evaluated, found be an excellent maximum TOF 19.8 min −1 .

Язык: Английский

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Activated Mn‐MACHO Complexes Form Stable CO₂ Adducts

Chemistry - A European Journal, Год журнала: 2023, Номер 30(9)

Опубликована: Ноя. 30, 2023

Manganese(I) carbonyl complexes bearing a MACHO-type ligand (HN(CH

Язык: Английский

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Impact of the Local Environment of Amines on the Activity for CO₂ Hydrogenation over Bifunctional Basic – Metallic Catalysts

ChemCatChem, Год журнала: 2022, Номер 14(18)

Опубликована: Июль 20, 2022

Abstract Bifunctional basic‐metallic catalysts proved to be efficient for the selective hydrogenation of CO 2 methanol. The activity these depends on cooperative interaction between amine groups and metallic sites, which is a function group density, Pd particle perimeter length geometric properties support pores. pore width has highest effect activity, increasing methanol yield by about half an order magnitude. Confining space leads three‐dimensional utilization available metal surface sites compared two‐dimensional distribution bifunctional in larger pores, where diameter decisive factor catalytic properties.

Язык: Английский

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Precapture of CO₂ and Hydrogenation into Methanol on Heterogenized Ruthenium and Amine‐Rich Catalytic Systems

ChemistryOpen, Год журнала: 2023, Номер 12(6)

Опубликована: Май 31, 2023

Abstract A heterogenized alternative to the homogeneous precapture of CO 2 with amines and subsequent hydrogenation MeOH was developed using aminated silica a Ru‐MACHO TM catalyst. Commercial mesoporous modified three different amino‐silane monomers used as support for Ru These composites were studied by TEM solid‐state NMR spectroscopy before after catalytic reaction. reactions conducted at 155 °C H pressures 75 bar, respectively, heterogeneous system (gas‐solid) being probed gas‐phase infrared quantify resulting products. High turnover number (TON) values observed samples secondary amines.

Язык: Английский

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