Synthesis of Polyethyleneimines from the Manganese‐Catalysed Coupling of Ethylene Glycol and Ethylenediamine DOI Creative Commons
Claire N. Brodie,

Aniekan E. Owen,

Julian Kolb

et al.

Angewandte Chemie, Journal Year: 2023, Volume and Issue: 135(29)

Published: May 17, 2023

Abstract Polyethyleneimines find many applications in products such as detergents, adhesives, cosmetics, and for processes tissue culture, gene therapy, CO 2 capture. The current state‐of‐the‐art technology the production of branched polyethyleneimines involves aziridine feedstock which is a highly toxic, volatile mutagenic chemical raises significant concern to human health environment. We report here novel method synthesis polyethyleneimine derivative from ethylene glycol ethylenediamine are much safer, environmentally benign, commercially available potentially renewable feedstock. polymerisation reaction catalysed by complex an earth‐abundant metal, manganese liberates H O only by‐product. Our mechanistic studies using combination DFT computation experiment suggest that proceeds formation subsequent hydrogenation imine intermediates.

Language: Английский

Divergent Synthesis of Alcohols and Ketones via Cross‐Coupling of Secondary Alcohols under Manganese Catalysis DOI

Feixiang Sun,

Jiamin Huang,

Zhihong Wei

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)

Published: April 21, 2023

A homogeneous manganese-catalyzed cross-coupling of two secondary alcohols for the divergent synthesis γ-disubstituted and β-disubstituted ketones is reported. Employing well-defined Mn-MACHOPh as catalyst, this novel protocol has a broad substrate scope with good functional group tolerance affords diverse library valuable disubstituted in moderate to yields. The strong influence reaction temperature on selective formation alcohol products was theorized preliminary DFT studies. Studies have shown that Gibbs free energy thermodynamically more favourable than corresponding at lower temperature.

Language: Английский

Citations

31

Synergism of Hydrogen-Induced Interstitial Effect and Gold-Induced Alloying Effect in PdAuH Metallene for Urea Electrosynthesis from Nitrate and Carbon Dioxide DOI
You Xu, Junjie Wang,

Youwei Sheng

et al.

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 8, 2025

Urea is a common agricultural fertilizer and industrial raw material, but at present, the traditional production of urea energy-and pollution-intensive. Electrocatalytic coupling CO2 ubiquitous nitrogen sources to synthesize considered as promising alternative method requiring high-performance catalysts boost C–N electrocatalysis process. Herein, hydrogen-intercalated Pd–Au bimetallene (PdAuHene) was prepared by three-step used for electrosynthesis from NO3– CO2, deriving an optimum Faradaic efficiency 33.88% yield rate 6.68 mmol g–1 h–1 applied potential −0.6 V vs RHE. Detailed material characterizations electrochemical studies reveal that metallene structure with ultrathin thickness could improve atomic utilization precious metal atoms, introduction Au H atoms adjust electronic Pd regulate evolution pathway key N-/C-intermediates, promote form urea.

Language: Английский

Citations

1

Synthesis of Polyethyleneimines from the Manganese‐Catalysed Coupling of Ethylene Glycol and Ethylenediamine DOI Creative Commons
Claire N. Brodie,

Aniekan E. Owen,

Julian Kolb

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)

Published: May 17, 2023

Polyethyleneimines find many applications in products such as detergents, adhesives, cosmetics, and for processes tissue culture, gene therapy, CO

Language: Английский

Citations

21

Formation of ylidenehydrazines enabled by manganese-catalyzed acceptorless dehydrogenative coupling DOI Creative Commons

Fangchao Wang,

Ding Ding,

Chunyan Zhang

et al.

Organic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(5), P. 1420 - 1429

Published: Jan. 1, 2024

A practical one-pot Mn-catalyzed tandem dehydrogenative condensation coupling of alcohols with hydrazines and halides to form ylidenehydrazines via an acceptorless strategy is reported.

Language: Английский

Citations

7

Unravelling a bench-stable zinc-amide compound as highly active multitasking catalyst for radical-mediated selective alk(en)ylation of unactivated carbocycles under mild conditions DOI Creative Commons

Sangita Sahoo,

Subarna Manna,

Arnab Rit

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(14), P. 5238 - 5247

Published: Jan. 1, 2024

The direct functionalization of unactivated organic moieties

Language: Английский

Citations

6

Direct Synthesis of Polyesterether from Ethylene Glycol DOI Creative Commons
Garima Saini, Pavel S. Kulyabin,

Angus McLuskie

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: April 8, 2025

We report here a method for making polyesterether from ethylene glycol. The reaction is catalyzed by ruthenium complex and liberates H2 gas H2O as byproducts. Mechanistic studies conducted through experiments DFT computations suggest that the chain growth of polymerization process involves both dehydrogenation dehydration pathways stemming hemiacetal intermediate, leading to formation esters ethers, respectively. Investigations into other diols have also been conducted, showing with lower number carbons between alcohol groups (propylene glycol, glycerol, 1,3-propanediol) lead whereas α,ω-diols containing higher (1,6-hexanediol 1,10-decanediol) polyester.

Language: Английский

Citations

0

Aiming at durable flame retardancy, smoke suppression, and qualified mechanical properties of polyurea by using surface-treated aluminum hypophosphite and interface-regulated MXene DOI

Qinyong Liu,

Jingfan Zhang,

Ximei Wen

et al.

Composites Communications, Journal Year: 2025, Volume and Issue: unknown, P. 102259 - 102259

Published: Jan. 1, 2025

Language: Английский

Citations

0

Rising Opportunities in Catalytic Dehydrogenative Polymerization DOI Creative Commons
Alejandra Sophia Lozano Pérez, Pavel S. Kulyabin, Amit Kumar

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(5), P. 3619 - 3635

Published: Feb. 13, 2025

This article gives a perspective on various types of catalytic dehydrogenative polymerization reactions (including organic and main group polymers) while introducing "hydrogen-borrowing polymerization" "acceptorless to this class. Limitations future opportunities each method have been discussed.

Language: Английский

Citations

0

Quaternary Medium-Entropy Alloy Metallene with Strong Charge Polarization for Highly Selective Urea Electrosynthesis from Carbon Dioxide and Nitrate DOI
Yuanbo Zhou, Mengfan Wang, Lifang Zhang

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 14, 2025

Electrochemical urea synthesis via the coreduction of CO2 and NO3- is a sustainable alternative to traditional Bosch-Meiser process. However, sluggish reaction kinetics usually result in low efficiency. Herein, we designed kind quaternary PdCuCoZn medium-entropy alloy (MEA) metallene for highly selective electrosynthesis. The random occupation Cu, Co, Zn with lower electronegativity face-centered cubic lattice Pd-based enables abundant electron donation from transition metals adjacent Pd atoms, leading formation charge-polarized Pdδ--Cu/Co/Znδ+ sites. Considering that pivotal C- N-intermediates, namely, *CO *NH2, are electrophilic nucleophilic, respectively, such strong charge polarization would greatly benefit their respective stabilization. stable adsorption bonded electron-rich sites *NH2 electron-deficient Cu/Co/Zn-based demonstrated by combination situ characterizations theoretical calculations. proof-of-concept MEA achieves maximum yield rate 1840 μg h-1 mg-1 high Faradaic efficiency 70.2%, surpassing most reported state-of-the-arts. Our strategy proposed this work believed enlighten design an effective catalyst used multistep reactions.

Language: Английский

Citations

0

Efficient N-Methylation of Primary Amides Using Methanol Under Mn(I)-Catalysis DOI

Reshma Babu,

Smruti Reka Pathy,

Ekambaram Balaraman

et al.

Tetrahedron, Journal Year: 2025, Volume and Issue: unknown, P. 134535 - 134535

Published: Feb. 1, 2025

Language: Английский

Citations

0