PMID- 37903133
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20231212
IS  - 1521-3773 (Electronic)
IS  - 1433-7851 (Linking)
VI  - 62
IP  - 51
DP  - 2023 Dec 18
TI  - Thermally Robust yet Deconstructable and Chemically Recyclable High-Density 
      Polyethylene (HDPE)-Like Materials Based on Si-O Bonds.
PG  - e202315085
LID - 10.1002/anie.202315085 [doi]
AB  - Polyethylene (PE) is the most widely produced synthetic polymer. By installing 
      chemically cleavable bonds into the backbone of PE, it is possible to produce 
      chemically deconstructable PE derivatives; to date, however, such designs have 
      primarily relied on carbonyl- and olefin-related functional groups. Bifunctional 
      silyl ethers (BSEs; SiR(2) (OR'(2) )) could expand the functional scope of PE 
      mimics as they possess strong Si-O bonds and facile chemical tunability. Here, we 
      report BSE-containing high-density polyethylene (HDPE)-like materials synthesized 
      through a one-pot catalytic ring-opening metathesis polymerization (ROMP) and 
      hydrogenation sequence. The crystallinity of these materials can be adjusted by 
      varying the BSE concentration or the steric bulk of the Si-substituents, 
      providing handles to control thermomechanical properties. Two methods for 
      chemical recycling of HDPE mimics are introduced, including a circular approach 
      that leverages acid-catalyzed Si-O bond exchange with 1-propanol. Additionally, 
      despite the fact that the starting HDPE mimics were synthesized by chain-growth 
      polymerization (ROMP), we show that it is possible to recover the molar mass and 
      dispersity of recycled HDPE products using step-growth Si-O bond formation or 
      exchange, generating high molecular weight recycled HDPE products with mechanical 
      properties similar to commercial HDPE.
CI  - (c) 2023 The Authors. Angewandte Chemie International Edition published by 
      Wiley-VCH GmbH.
FAU - Johnson, Alayna M
AU  - Johnson AM
AUID- ORCID: 0000-0003-4305-2495
AD  - Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts 
      Avenue, Cambridge, MA 02139, USA.
FAU - Johnson, Jeremiah A
AU  - Johnson JA
AUID- ORCID: 0000-0001-9157-6491
AD  - Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts 
      Avenue, Cambridge, MA 02139, USA.
LA  - eng
GR  - 2116298/Division of Chemistry/
PT  - Journal Article
DEP - 20231115
PL  - Germany
TA  - Angew Chem Int Ed Engl
JT  - Angewandte Chemie (International ed. in English)
JID - 0370543
SB  - IM
OTO - NOTNLM
OT  - Closed Loop Recycling
OT  - Green Chemistry
OT  - Polyethylene Mimic
OT  - Ring-Opening Polymerization
OT  - Silyl Ether
EDAT- 2023/10/30 18:42
MHDA- 2023/10/30 18:43
CRDT- 2023/10/30 13:44
PHST- 2023/10/07 00:00 [received]
PHST- 2023/10/30 18:43 [medline]
PHST- 2023/10/30 18:42 [pubmed]
PHST- 2023/10/30 13:44 [entrez]
AID - 10.1002/anie.202315085 [doi]
PST - ppublish
SO  - Angew Chem Int Ed Engl. 2023 Dec 18;62(51):e202315085. doi: 
      10.1002/anie.202315085. Epub 2023 Nov 15.