Polyethylene materials are highly important polymers which are produced in the largest volume among all plastics. Due to the chemical inert property of saturated carbon-carbon bonds, the degradation of polyethylene is extremely challenging, which prevents them from efficient chemical recycling. Installing functional groups in the main chain of polyethylenes may facilitate the degradation and following chemical recycling of polyethylene materials. Here we report a highly selective approach for the synthesis of high density polyethylenes bearing low content isolated in-chain carbonyls. Linear high-molecular weight polyethylene chains are synthesized via the palladium catalyzed copolymerization of ethylene with metal carbonyls. Different from traditional ethylene/CO copolymerization reactions, excellent non-alternating selectivity has been achieved. While the properties of polyethylene have been retained in the copolymer, faster degradation compared with that of polyethylene was observed upon UV light irradiation. The synthesized materials may therefore serve as more environmentally friendly alternative plastics than traditional polyethylene materials.

/pdf/high-density-polyethylenes-bearing-isolated-in-chain-1l1k02b9x8.pdf

High Density Polyethylenes Bearing Isolated In-Chain Carbonyls.

Carbon dioxide (CO2) has long been recognized as an ideal C1 feedstock comonomer for producing sustainable materials because it is renewable, abundant, and cost-effective. However, activating CO2 presents a significant challenge because it is highly oxidized and stable. A CO2/butadiene-derived δ-valerolactone (EVP), generated via palladium-catalyzed telomerization between CO2 and butadiene, has emerged as an attractive intermediate for producing sustainable copolymers from CO2 and butadiene. Owing to the presence of two active carbon-carbon double bonds and a lactone unit, EVP serves as a versatile intermediate for creating sustainable copolymers with a CO2 content of up to 29 wt % (33 mol %). In this Review, advances in the synthesis of copolymers from CO2 and butadiene with divergent structures through various polymerization protocols have been summarized. Achievements made in homo- and copolymerization of EVP or its derivatives are comprehensively reviewed, while the postmodification of the obtained copolymers to access new polymers are also discussed. Meanwhile, potential applications of the obtained copolymers are also discussed. The literature references were sorted into sections based on polymerization strategies and mechanisms, facilitating readers in gaining a comprehensive view of the present chemistry landscape and inspiring innovative approaches to synthesizing novel CO2-derived copolymers.

Sustainable Copolymer Synthesis from Carbon Dioxide and Butadiene.

Abstract The perfect alternating CO/olefin copolymers constitute an important class of new materials. Their synthesis requires a catalyst; in general, the applied catalytic systems are formed by a palladium(II) salt, modified by diphosphine or dinitrogen chelating ligands, in the presence of a BrOnsted acid as cocatalyst and, frequently, an oxidant such as 1,4-benzoquinone. Alcoholic medium is generally preferred. This overview will report on the main catalytic systems based on bidentate nitrogen-donor chelating ligands; particular attention will be dedicated to the CO/styrene copolymerization. A detailed analysis of several parameters influencing the yield and the quality of CO/styrene polyketone will be presented, together with the discussion of the control of the stereochemistry of the insertion of styrene in the growing chain.

Pd(II) complexes with bidentate nitrogen-donor chelating ligands: very versatile and active catalyst precursors for the CO/olefins co- and terpolymerization reactions

Water electrolysis is by far the most appealing method to produce green hydrogen. Among the possible technologies, Anion Exchange Membrane (AEM) water electrolyzers are promising in the medium term, as they make it possible to avoid critical and noble materials as catalyst components. However, AEMs are still lacking in performance and stability, which has become the current research focus. Here, we report the facile and inexpensive chemical modification of polyketone (PK) with a functional unit encompassing morpholinium as the positively charged group, and the fabrication of self-standing membranes. The synthesis products are investigated with an ensemble of physico-chemical and spectroscopic techniques, including solid-state and time-domain NMR, FT-IR, and thermal analysis. The membranes show good Ion Exchange Capacity values in the range 1.48–2.24 mmol g−1. A preliminary electrolysis test shows that the PK-based membrane has performance comparable to that of a commercial one. 

/pdf/morpholinium-modified-polyketone-based-anion-exchange-3fzfalil.pdf

Morpholinium‐Modified, Polyketone‐Based Anion Exchange Membranes for Water Electrolysis

Photo-Iniferter RAFT Synthesis of Versatile, Nonalternating Poly(acrylate-co-isocyanides)

Synthesis of polyketones by copolymerization of alkenes with carbon monoxide is reviewed. While radical copolymerization of ethylene and CO provides a copolymer with ethylene/CO > 1, metal-catalyzed copolymerization gives completely alternating copolymers with few exceptions. Applicable alkenes and their equivalents are described with proper metal catalysts, focusing on the control of polymer structures. Physical properties of the polymers are shown with a brief introduction for industrial applications.

Alkene/CO Copolymerization

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Alkene/CO Copolymerization