Efficient and selective approach to biomass-based amine by reductive amination of furfural using Ru catalyst

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 309, С. 121262 - 121262

Опубликована: Март 2, 2022

Язык: Английский

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Single-step conversion of wood lignin into phenolic amines

Chem, Год журнала: 2023, Номер 9(10), С. 2869 - 2880

Опубликована: Июнь 16, 2023

Язык: Английский

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Concepts Relevant for the Kinetic Analysis of Reversible Reaction Systems

Chemical Reviews, Год журнала: 2023, Номер 123(6), С. 2950 - 3006

Опубликована: Фев. 21, 2023

The net rate of a reversible chemical reaction is the difference between unidirectional rates traversal along forward and reverse paths. In multistep sequence, trajectories, in general, are not microscopic one another; rather, each route comprised distinct rate-controlling steps, intermediates, transition states. Consequently, traditional descriptors (e.g., orders) do reflect intrinsic kinetic information but instead conflate contributions determined by (i) occurrence forward/reverse reactions (i.e., kinetics) (ii) reversibility nonequilibrium thermodynamics). This review aims to provide comprehensive resource analytical conceptual tools which deconvolute kinetics thermodynamics disambiguate trajectories precisely identify rate- reversibility-controlling molecular species steps systems. extrication mechanistic from bidirectional accomplished through equation-based formalisms De Donder relations) grounded principles interpreted context theories developed past 25 years. aggregate mathematical detailed herein general thermochemical electrochemical encapsulates diverse body scientific literature encompassing physics, thermodynamics, kinetics, catalysis, modeling.

Язык: Английский

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Activity enhancement of Ru/CeO2 for N-alkylation of amines with alcohols through tailoring metal-support interaction

Journal of Catalysis, Год журнала: 2023, Номер 429, С. 115241 - 115241

Опубликована: Дек. 4, 2023

Язык: Английский

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Synergy between Ru and WO_x Enables Efficient Hydrodeoxygenation of Primary Amides to Amines

ACS Catalysis, Год журнала: 2022, Номер 12(11), С. 6302 - 6312

Опубликована: Май 12, 2022

The selective reduction of primary amides to the corresponding amines is a key reaction in both pharmaceutical chemistry and polymer industry; yet, it requires stoichiometric amount expensive environmentally unfriendly hydride reagents. Hydrodeoxygenation (HDO), on other hand, highly desired benign alternative; presents significant challenges activity selectivity control. In this work, we have developed bifunctional 2Ru1W/SiO2 catalyst, which afforded 93.6% conversion 83.7% amine after for 12 h HDO cyclohexanecarboxamide at 433 K, initial rate reached 48.2 h–1, 1 order magnitude higher than catalysts reported earlier. catalyst also presented excellent reusability substrate diversity. performances various Ru–W/SiO2 critically depend synergy between W Ru, with best performance accessible W/Ru atomic ratio 0.27. Characterizations kinetics revealed that Ru promoted W6+ W5+ via hydrogen spillover, resultant low-coordinated responsible activation C═O bond amide, leading almost zero respect amide much lower apparent energy over bimetallic contrast first Ru/SiO2. Nevertheless, ratios 0.27 resulted larger WOx domains valence states W, adsorbed so strongly surface was poisoned, dramatic decrease selectivity. strategy as well mechanism understanding work will provide insights into design used demanding chemical transformations.

Язык: Английский

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Catalytic reductive amination of furfural to furfurylamine on robust ultra-small Ni nanoparticles

Nano Research, Год журнала: 2022, Номер 16(3), С. 3719 - 3729

Опубликована: Сен. 21, 2022

Язык: Английский

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One-pot production of phenazine from lignin-derived catechol

Green Chemistry, Год журнала: 2021, Номер 24(3), С. 1224 - 1230

Опубликована: Дек. 22, 2021

Upgrading lignin-derived monomeric products is crucial in bio-refineries to effectively utilize lignin. Herein, we report a simple strategy convert catechol phenazine, useful N-heterocycle three-aromatic-ring compound, whose current synthetic procedure complex via petroleum-derived feedstock. The reaction uses as the sole carbon source and aqueous ammonia media nitrogen source. Without additional solvents, phenazine was obtained 67% yield form of high purity crystals (>97%) over Pd/C catalyst after one-pot-two-stage reaction. When cyclohexane used co-solvent first step, higher (81%) (>99%) were achieved. Mechanistic investigations involving control experiments an isotope labeling study reveal that hydrogenation, amination, coupling dehydrogenation reactions are key steps leading formation. conversion other catechols highlights protocol extendable produce substituted phenazines.

Язык: Английский

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Designed TiS₂ nanosheets for efficient electrocatalytic reductive amination of biomass-derived furfurals

Green Chemistry, Год журнала: 2022, Номер 24(24), С. 9570 - 9578

Опубликована: Янв. 1, 2022

Laminate TiS 2 nanosheets were successfully constructed for the electrochemical synthesis of valuable primary amines using biomass-derived furfurals at mild temperature and pressure.

Язык: Английский

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Paving the Way for Reductive Amination: Boosting Catalytic Ammonolysis of Schiff Base

ACS Catalysis, Год журнала: 2023, Номер 13(19), С. 13034 - 13042

Опубликована: Сен. 22, 2023

The synthesis of primary amines through reductive/hydrogen-borrowing amination has garnered significant attention due to their wide application in the chemical industry. key challenge reaction arises from two competing balances: hydrogenations imine versus Schiff base and ammonolysis hydrogenation base. former received extensive attention, latter, which directly determines selectivity amine, recently emerged as a fresh view for enhancing catalytic performance. Thus, gaining insights into promoting latter is becoming increasingly urgent catalyst design. This Perspective starts by presenting overall design principles mainly discusses influence balances on effective approaches tackle them. A profound emphasis placed advancing bases an in-depth understanding structure–activity relationships mechanisms. Finally, three directions deserving future investigations are provided. distinctive not only enhances importance comprehension amine but also unveils efficient avenues

Язык: Английский

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Coupling Cross-Dimensional Ru₁–Ru_n Sites in Confined Nanoislands to Overcome the Limitation of Coadsorption and Diffusion in Tandem Reactions

ACS Catalysis, Год журнала: 2024, Номер 14(3), С. 1584 - 1594

Опубликована: Янв. 16, 2024

Integrating different reaction sites offers prospects to address the difficulties in single-atom catalysis and helps overcome limitation of scaling relations for coadsorption. Here, we coupled dimensional Ru1 Run active on confined Co nanoislands reductive amination 5-hydroxymethylfurfural (5-HMF) 5-aminomethyl-2-furanyl alcohol (AMF), constrained by disequilibrium adsorption NH3/H2. Ru clusters trigger an ensemble effect multipoint-bonding with NH3 thus become more conductive dissociate NH2* than both thermodynamically kinetically, which releases activating H2 enhance local H* coverage. Furthermore, intimate spaces enable timely diffusion NH2*/H* react imine intermediates adsorbed di-σC,N configuration. With cross-dimensional overcoming limitations competitive diffusion, Ru1+n@Co/MMO exhibits a record-high AMF production rate (295 g·gRu–1 h–1) without requirement high NH3/H2 feeding, it mass specific activity even higher that Ru1@Co/MMO.

Язык: Английский

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