Selective Lanthanide‐Organic Catalyzed Depolymerization of Nylon‐6 to ϵ‐Caprolactam DOI Creative Commons
Lukas Wursthorn,

Kristen Beckett,

Jacob O. Rothbaum

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(4)

Published: Nov. 28, 2022

Nylon-6 is selectively depolymerized to the parent monomer ϵ-caprolactam by readily accessible and commercially available lanthanide trisamido catalysts Ln(N(TMS)2 )3 (Ln=lanthanide). The depolymerization process solvent-free, near quantitative, highly selective, operates at lowest temperature reported date. catalytic activity of different trisamides scales with Ln3+ ionic radius, this effective post-consumer as well Nylon-6+polyethylene, polypropylene or polyethylene terephthalate mixtures. Experimental kinetic data theoretical (DFT) mechanistic analyses suggest initial deprotonation a Nylon terminal amido N-H bond, which covalently binds catalyst polymer, followed chain-end back-biting in units are sequentially extruded from chain end.

Language: Английский

Chemical and biological catalysis for plastics recycling and upcycling DOI
Lucas D. Ellis, Nicholas A. Rorrer, Kevin P. Sullivan

et al.

Nature Catalysis, Journal Year: 2021, Volume and Issue: 4(7), P. 539 - 556

Published: July 22, 2021

Language: Английский

Citations

731

Homogeneous Catalysis for Sustainable Energy: Hydrogen and Methanol Economies, Fuels from Biomass, and Related Topics DOI Creative Commons
Amit Kumar, Prosenjit Daw, David Milstein

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 122(1), P. 385 - 441

Published: Nov. 2, 2021

As the world pledges to significantly cut carbon emissions, demand for sustainable and clean energy has now become more important than ever. This includes both production storage of carriers, a majority which involve catalytic reactions. article reviews recent developments homogeneous catalysts in emerging applications energy. The most focus been on hydrogen as several efficient have reported recently (de)hydrogenative transformations promising economy. Another direction that extensively covered this review is methanol Homogeneous investigated from CO

Language: Английский

Citations

418

Chemically recyclable thermoplastics from reversible-deactivation polymerization of cyclic acetals DOI
Brooks A. Abel, Rachel L. Snyder, Geoffrey W. Coates

et al.

Science, Journal Year: 2021, Volume and Issue: 373(6556), P. 783 - 789

Published: Aug. 12, 2021

Identifying plastics capable of chemical recycling to monomer (CRM) is the foremost challenge in creating a sustainable circular plastic economy. Polyacetals are promising candidates for CRM but lack useful tensile strengths owing low molecular weights produced using current uncontrolled cationic ring-opening polymerization (CROP) methods. Here, we present reversible-deactivation CROP cyclic acetals commercial halomethyl ether initiator and an indium(III) bromide catalyst. Using this method, synthesize poly(1,3-dioxolane) (PDXL), which demonstrates strength comparable some commodity polyolefins. Depolymerization PDXL strong acid catalysts returns near-quantitative yield even proceeds from waste mixture. Our efficient method affords tough thermoplastic that can undergo selective depolymerization monomer.

Language: Английский

Citations

350

A unified view on catalytic conversion of biomass and waste plastics DOI Open Access
Kyungho Lee, Yaxuan Jing, Yanqin Wang

et al.

Nature Reviews Chemistry, Journal Year: 2022, Volume and Issue: 6(9), P. 635 - 652

Published: Aug. 11, 2022

Language: Английский

Citations

344

Enzymes’ Power for Plastics Degradation DOI
Vincent Tournier, Sophie Duquesne,

Frédérique Guillamot

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 5612 - 5701

Published: March 14, 2023

Plastics are everywhere in our modern way of living, and their production keeps increasing every year, causing major environmental concerns. Nowadays, the end-of-life management involves accumulation landfills, incineration, recycling to a lower extent. This ecological threat environment is inspiring alternative bio-based solutions for plastic waste treatment toward circular economy. Over past decade, considerable efforts have been made degrade commodity plastics using biocatalytic approaches. Here, we provide comprehensive review on recent advances enzyme-based biocatalysis design related processes recycle or upcycle plastics, including polyesters, polyamides, polyurethanes, polyolefins. We also discuss scope limitations, challenges, opportunities this field research. An important message from that polymer-assimilating enzymes very likely part solution reaching

Language: Английский

Citations

285

Upcycling and catalytic degradation of plastic wastes DOI Creative Commons
Qidong Hou,

Meinan Zhen,

Hengli Qian

et al.

Cell Reports Physical Science, Journal Year: 2021, Volume and Issue: 2(8), P. 100514 - 100514

Published: July 22, 2021

Various recycling technologies have been developed to deal with plastic problems, but they face considerable economic and technological challenges in practice. An attractive alternative is upcycling, which aims dig out the embedded value incentivize large-scale valorization of wastes. The degradation nonrecoverable wastes another necessity treat omnipresent pollution. This review presents an overview on conversion toward value-added products catalytic Based examination traditional products, we summarize state-of-the-art design development high-value high-performance fuels, chemicals, materials. Subsequently, highlight advances plastics environmentally benign or degradable mineralization into carbon dioxide water. We conclude our perspective ongoing challenge opportunities.

Language: Английский

Citations

241

Microplastics remediation in aqueous systems: Strategies and technologies DOI

Kunsheng Hu,

Wenjie Tian, Yangyang Yang

et al.

Water Research, Journal Year: 2021, Volume and Issue: 198, P. 117144 - 117144

Published: April 15, 2021

Language: Английский

Citations

145

Catalytic strategies for upvaluing plastic wastes DOI Creative Commons
Meiqi Zhang, Meng Wang, Bo Sun

et al.

Chem, Journal Year: 2022, Volume and Issue: 8(11), P. 2912 - 2923

Published: Sept. 7, 2022

Language: Английский

Citations

124

A circular polyester platform based on simple gem-disubstituted valerolactones DOI
Xinlei Li, Ryan W. Clarke,

Jingyang Jiang

et al.

Nature Chemistry, Journal Year: 2022, Volume and Issue: 15(2), P. 278 - 285

Published: Nov. 7, 2022

Language: Английский

Citations

110

Redesigned Hybrid Nylons with Optical Clarity and Chemical Recyclability DOI
Robin M. Cywar, Nicholas A. Rorrer, Heather B. Mayes

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(12), P. 5366 - 5376

Published: March 15, 2022

Aliphatic polyamides, or nylons, are typically highly crystalline and thermally robust polymers used in high-performance applications. Nylon 6, a high-ceiling-temperature (HCT) polyamide from ε-caprolactam, lacks expedient chemical recyclability, while low-ceiling temperature (LCT) nylon 4 pyrrolidone exhibits complete but it is unstable not melt-processable. Here, we introduce hybrid nylon, 4/6, based on bicyclic lactam composed of both HCT ε-caprolactam LCT motifs hybridized offspring structure. Hybrid 4/6 overcomes trade-offs (de)polymerizability performance properties the parent exhibiting excellent polymerization facile depolymerization characteristics. This stereoregular forms nanocrystalline domains, allowing optical clarity high thermal stability, however, without displaying melting transition before decomposition. Of series statistical copolymers comprising 4, 50/50 copolymer achieves greatest synergy reactivity polymer each homopolymer, offering an amorphous with favorable properties, including clarity, glass temperature, melt processability, full recyclability.

Language: Английский

Citations

88