Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Mechanochemically accelerated deconstruction of chemically recyclable plastics

Journal Article · · Science Advances
 [1];  [2];  [1];  [3];  [1];  [4];  [1];  [5];  [5];  [1];  [5];  [2];  [1]
  1. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. University of California, Berkeley, CA (United States)
  4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
  5. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)

Plastics redesign for circularity has primarily focused on monomer chemistries enabling faster deconstruction rates concomitant with high monomer yields. Yet, during deconstruction, polymer chains interact with their reaction medium, which remains underexplored in polymer reactivity. Here, we show that, when plastics are deconstructed in reaction media that promote swelling, initial rates are accelerated by over sixfold beyond those in small-molecule analogs. This unexpected acceleration is primarily tied to mechanochemical activation of strained polymer chains; however, changes in the activity of water under polymer confinement and bond activation in solvent-separated ion pairs are also important. Together, deconstruction times can be shortened by seven times by codesigning plastics and their deconstruction processes.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
2476944
Journal Information:
Science Advances, Journal Name: Science Advances Journal Issue: 38 Vol. 10; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English

References (56)

Merck molecular force field. I. Basis, form, scope, parameterization, and performance of MMFF94 journal April 1996
Healable, Recyclable, and Mechanically Tough Polyurethane Elastomers with Exceptional Damage Tolerance journal November 2020
The ozone attack on swollen elastomeric networks journal October 1969
Ozone attack on rubber vulcanizates journal January 1956
On the limited memory BFGS method for large scale optimization journal August 1989
Time-dependent density functional theory within the Tamm–Dancoff approximation journal December 1999
Bulk depolymerization of poly(methyl methacrylate) via chain-end initiation for catalyst-free reversion to monomer journal September 2023
Bioinspired Multifunctional Anti-icing Hydrogel journal March 2020
Improved cardanol derived epoxy coatings journal February 2016
The Raman OH stretching bands of liquid water journal November 2009
Polydiketoenamines for a Circular Plastics Economy journal September 2022
In Situ / Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy journal September 2020
Development and Benchmarking of Open Force Field 2.0.0: The Sage Small Molecule Force Field journal May 2023
Semiempirical Modeling of Ag Nanoclusters: New Parameters for Optical Property Studies Enable Determination of Double Excitation Contributions to Plasmonic Excitation journal June 2016
Unified Efficient Thermostat Scheme for the Canonical Ensemble with Holonomic or Isokinetic Constraints via Molecular Dynamics journal May 2019
Ion-Specific Interfacial Crystallization of Polymer-Grafted Nanoparticles journal July 2017
Charge Scaling Manifesto: A Way of Reconciling the Inherently Macroscopic and Microscopic Natures of Molecular Simulations journal November 2019
Swelling-Activated, Soft Mechanochemistry in Polymer Materials journal February 2023
Tuning Ice Nucleation and Propagation with Counterions on Multilayer Hydrogels journal September 2018
Swelling Dynamics of a Disk-Shaped Gel journal May 2021
Mechanical Acceleration of Ester Bond Hydrolysis in Polymers journal November 2022
Rational Design of Chemical Catalysis for Plastic Recycling journal April 2022
Circular Polydiketoenamine Elastomers with Exceptional Creep Resistance via Multivalent Cross-Linker Design journal November 2023
OpenMM 4: A Reusable, Extensible, Hardware Independent Library for High Performance Molecular Simulation journal November 2012
Cation-Water Interactions: The M+(H2O)n Clusters for Alkali Metals, M = Li, Na, K, Rb, and Cs journal March 1995
Specific Ion Effects on the Water Solubility of Macromolecules:  PNIPAM and the Hofmeister Series journal October 2005
Specific Ion Effects on Interfacial Water Structure near Macromolecules journal October 2007
Structure of Hydronium (H 3 O + )/Chloride (Cl ) Contact Ion Pairs in Aqueous Hydrochloric Acid Solution: A Zundel-like Local Configuration journal September 2010
Variable Amine Spacing Determines Depolymerization Rate in Polydiketoenamines journal March 2023
Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide journal August 2017
Molecular Scale Solvation in Complex Solutions journal July 2019
How Ions Affect the Structure of Water: A Combined Raman Spectroscopy and Multivariate Curve Resolution Study journal December 2013
Solvent Swelling Activation of a Mechanophore in a Polymer Network journal April 2014
Ion-specific ice recrystallization provides a facile approach for the fabrication of porous materials journal May 2017
Forcing the reversibility of a mechanochemical reaction journal August 2018
Closed-loop recycling of plastics enabled by dynamic covalent diketoenamine bonds journal April 2019
Olefin metathesis-based chemically recyclable polymers enabled by fused-ring monomers journal July 2021
Sustainable polyesters via direct functionalization of lignocellulosic sugars journal June 2022
Chemical recycling to monomer for an ideal, circular polymer economy journal April 2020
Closed-loop recycling of polyethylene-like materials journal February 2021
Strong tough hydrogels via the synergy of freeze-casting and salting out journal February 2021
In situ Raman spectroscopy reveals the structure and dissociation of interfacial water journal December 2021
Biorenewable and circular polydiketoenamine plastics journal July 2023
Chemical and biological catalysis for plastics recycling and upcycling journal July 2021
Promoting Cu-catalysed CO2 electroreduction to multicarbon products by tuning the activity of H2O journal August 2023
Activity of water in aqueous systems; A frequently neglected property journal January 2005
Time-dependent density functional theory calculations of near-edge X-ray absorption fine structure with short-range corrected functionals journal January 2009
Comparison of simple potential functions for simulating liquid water journal July 1983
Software for the frontiers of quantum chemistry: An overview of developments in the Q-Chem 5 package journal August 2021
Tuning ice nucleation with counterions on polyelectrolyte brush surfaces journal June 2016
Circularity in mixed-plastic chemical recycling enabled by variable rates of polydiketoenamine hydrolysis journal July 2022
Chemically recyclable thermoplastics from reversible-deactivation polymerization of cyclic acetals journal August 2021
Chemically circular, mechanically tough, and melt-processable polyhydroxyalkanoates journal April 2023
SolvationAnalysis: A Python toolkit for understanding liquid solvation structure in classical molecular dynamics simulations journal April 2023
MDAnalysis: A Python Package for the Rapid Analysis of Molecular Dynamics Simulations conference January 2016
Vibrational Raman Spectroscopy of the Hydration Shell of Ions journal December 2022

Similar Records

Magnetic resonance insights into the heterogeneous, fractal-like kinetics of chemically recyclable polymers
Journal Article · Wed Apr 03 00:00:00 EDT 2024 · Science Advances · OSTI ID:2448501

Selective deconstruction of mixed plastics by a tailored organocatalyst
Journal Article · Tue Aug 29 00:00:00 EDT 2023 · Materials Horizons · OSTI ID:1992142