Green Carbon Science: Efficient Carbon Resource Processing, Utilization, and Recycling towards Carbon Neutrality

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 61(15)

Published: Dec. 17, 2021

Green carbon science is defined as the "study and optimization of transformation carbon-containing compounds relevant processes involved in entire cycle from resource processing, energy utilization, CO2 fixation, recycling to utilize resources efficiently minimize net emission."[1] related closely neutrality, fields have developed quickly last decade. In this Minireview, we propose concept index, recent progress petroleum refining, production liquid fuels, chemicals, materials using coal, methane, , biomass, waste plastics highlighted combination with green science. An outlook for these important provided final section.

Language: Английский

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Highly Efficient Conversion of Propargylic Alcohols and Propargylic Amines with CO₂ Activated by Noble‐Metal‐Free Catalyst Cu₂O@ZIF‐8

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(19)

Published: Jan. 11, 2022

The cyclization reactions of propargylic alcohols and amines with CO2 are important in industrial applications, but it was a great challenge that non-noble-metal catalysts catalyzed both under mild conditions. Herein, the catalyst Cu2 O@ZIF-8 prepared by encapsulating O nanoparticles into robust ZIF-8, can effectively catalyze valuable α-alkylidene cyclic carbonates oxazolidinones turnover numbers (TONs) 12.1 19.6, which be recycled at least five times. mechanisms were further uncovered NMR, FTIR, 13 C isotope-labeling experiments DFT calculations, DBU synergistically activate C≡C bond hydroxy/amino group substrates. Importantly, is first example noble-metal-free simultaneously.

Language: Английский

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Recent progress in CO₂ conversion into organic chemicals by molecular catalysis

Green Chemistry, Journal Year: 2023, Volume and Issue: 25(17), P. 6538 - 6560

Published: Jan. 1, 2023

An activation toolbox for the effective catalytic conversion of CO 2 to chemicals is proposed along with challenges and prospects related future development this exciting technology.

Language: Английский

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Recent advances in asymmetric synthesis with CO2

Science China Chemistry, Journal Year: 2020, Volume and Issue: 63(10), P. 1336 - 1351

Published: July 20, 2020

Language: Английский

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From CO₂ activation to catalytic reduction: a metal-free approach

Chemical Science, Journal Year: 2020, Volume and Issue: 11(39), P. 10571 - 10593

Published: Jan. 1, 2020

This review article documents the key developments in metal-free catalytic reduction of CO₂ into various energy intensive chemicals and fuels, reductive functionalization for formation new C–N bonds.

Language: Английский

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A NHC-Silyliumylidene Cation for Catalytic N-Formylation of Amines Using Carbon Dioxide

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(24), P. 14824 - 14833

Published: Dec. 3, 2020

This study describes the use of a silicon(II) complex, namely, NHC-silyliumylidene cation complex [(IMe)2SiH]I (1, IMe = :C{N(Me)C(Me)}2), to catalyze chemoselective N-formylation primary and secondary amines using CO2 PhSiH3 under mild conditions afford corresponding formamides as sole product (average reaction time: 4.5 h; amines, average yield: 95%, TOF: 8 h–1; 98%, 17 h–1). The activity 1 yields outperform currently available non-transition-metal catalysts used for this catalysis. Mechanistic studies show that center in catalyzes C–N bond formation via different pathway comparison with catalysts. It sequentially activates CO2, PhSiH3, which proceeds dihydrogen elimination mechanism, form formamides, siloxanes, gas.

Language: Английский

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Green Carbon Science: Efficient Carbon Resource Processing, Utilization, and Recycling towards Carbon Neutrality

Angewandte Chemie, Journal Year: 2021, Volume and Issue: 134(15)

Published: Dec. 17, 2021

Abstract Green carbon science is defined as the “study and optimization of transformation carbon‐containing compounds relevant processes involved in entire cycle from resource processing, energy utilization, CO 2 fixation, recycling to utilize resources efficiently minimize net emission.” [1] related closely neutrality, fields have developed quickly last decade. In this Minireview, we propose concept index, recent progress petroleum refining, production liquid fuels, chemicals, materials using coal, methane, , biomass, waste plastics highlighted combination with green science. An outlook for these important provided final section.

Language: Английский

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A Porous Copper–Organic Framework Assembled by [Cu₁₂] Nanocages: Highly Efficient CO₂ Capture and Chemical Fixation and Theoretical DFT Calculations

Inorganic Chemistry, Journal Year: 2021, Volume and Issue: 60(12), P. 9122 - 9131

Published: June 1, 2021

A new porous copper–organic framework assembled from 12-nuclear [Cu12] nanocages {[Cu2(L4–)(H2O)2]·4DMA·2H2O}n (1) (H4L = 5,5′-(butane-1,4-diyl)-bis(oxy)-diisophthalic acid) was successfully prepared and structurally characterized. Compound 1 feathering of a 3D with two types 1D nanotubular channels large specific surface area can effectively enrich various harmful dyes. Additionally, due to the carbon dioxide (CO2) interactions open Cu(II) sites electron-rich ether oxygen atoms ligand in 1, it exhibits highly selective CO2 uptake. Interestingly, catalyze cycloaddition reaction epoxides under mild conditions, which is ascribed Lewis acid 1. Importantly, acting as heterogeneous catalyst be recycled at least 10 times without an obvious loss catalytic activity, mechanism further uncovered by density functional theory (DFT) calculations. This study greatly MOF catalysts system conversion also provide valuable guidance for design efficient MOFs catalysts.

Language: Английский

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Tailoring Active Cu₂O/Copper Interface Sites for N‐Formylation of Aliphatic Primary Amines with CO₂/H₂

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(21)

Published: March 23, 2023

Heterogeneously catalyzed N-formylation of amines to formamide with CO2 /H2 is highly attractive for the valorization . However, relationship catalytic performance catalyst structure still elusive. Herein, mixed valence catalysts containing Cu2 O/Cu interface sites were constructed this transformation. Both aliphatic primary and secondary diverse structures efficiently converted into desired formamides good excellent yields. Combined ex in situ characterization revealed that presence was vital activity. Density functional theory (DFT) calculations demonstrated better activity O/Cu(111) than Cu(111) attributed assistance oxygen at (Ointer ) formation Ointer -H moieties, which not only reduce apparent barrier HCOOH but also benefit desorption N-formylated amine, leading high selectivity.

Language: Английский

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Ruthenium Single-Atom Anchored in Polyoxometalate-Ionic Liquids for N-Formylation of Amines with CO₂ and H₂

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(15), P. 10295 - 10308

Published: July 24, 2023

In this work, we have developed a Ru single-atom substituted polyoxometalate-based ionic liquid ([TOMA6SiW11O39Ru(dmso)], TOMA = methyltrioctylammonium, named as Ru-POM-IL) and confirmed that the is anchored into framework of POM. The binary (IL) system, composed POM-based IL 1-butyl-3-methyl-imidazolium acetate (BMImOAc), exhibits high efficiency for N-formylation amines with CO2 H2, leading to formylamides yields in toluene-IL biphasic media. characterization by laser confocal scanning microscopy reveals specific sponge-like structure IL, facilitating efficient contact between catalytic active sites substrate molecules. Detailed investigations elucidate reaction proceeds via pathway formate intermediates, including adsorption activation BMImOAc, morpholine-assisted heterolytic splitting H2 Ru–Hδ- species Hδ+ attachment morpholine N center; coupling afford species; then dehydration intermediates formamides. system offered advantages efficiency, robustness, recyclability reaction.

Language: Английский

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