Spatially resolved reaction environments in mechanochemical upcycling of polymers

Kinga Gołąbek; Yuchen Chang; Lauren R. Mellinger; Mariana V. Rodrigues; Cauê de Souza Coutinho Nogueira; Fabio B. Passos; Yutao Xing; Aline Ribeiro Passos; Mohammed H. Saffarini; Austin B. Isner; David S. Sholl; Carsten Sievers

doi:10.1016/j.chempr.2025.102754

Spatially resolved reaction environments in mechanochemical upcycling of polymers

Kinga Gołąbek
, Yuchen Chang
, Lauren R. Mellinger
, Mariana V. Rodrigues
, Cauê de Souza Coutinho Nogueira
, Fabio B. Passos
, Yutao Xing
, Aline Ribeiro Passos
, Mohammed H. Saffarini
, Austin B. Isner
, David S. Sholl
, Carsten Sievers

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

Mechanochemical processing is an attractive and scalable approach for the upcycling of polymers. The complex and dynamic environment in ball milling, however, makes gaining insight into the physicochemical nature of the collisions driving mechanochemistry challenging, which, in turn, hampers the optimization of these processes. We used controlled single impacts followed by multiple spatially resolved analytical methods (focused ion beam microscopy, Raman spectro-microscopy, and small-angle X-ray scattering) and material point method simulations to gain unprecedented information about mechanochemical depolymerization of poly(ethylene terephthalate). These measurements highlight the contributions of plastic deformation, amorphization, and depolymerization during the transfer of kinetic energy in collisions relevant to ball mills and will enable reactor models based on fundamental kinetics.

Original language	English
Article number	102754
Journal	Chem
Volume	12
Issue number	1
DOIs	https://doi.org/10.1016/j.chempr.2025.102754
State	Published - Jan 15 2026

Funding

K.G., Y.C., L.R.M., and C.S. were supported by the US National Science Foundation grant 2028998 . M.H.S., A.B.I., and D.S.S. were supported by the US Department of Energy, Office of Science, Energy Earthshot Initiative, as part of the NEETER EERC grant KC0315010 and US Department of Energy, US Department of Energy contract DE-AC05-00OR22725 . The ORNL team used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory (ORNL), which is supported by the Office of Science of the US Department of Energy . M.V.R. was supported by Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) grant PCI-DA # 302036/2024-5 . This research used facilities of the Brazilian Synchrotron Light Laboratory (LNLS), part of the Brazilian Center for Research in Energy and Materials (CNPEM), a private non-profit organization under the supervision of the Brazilian Ministry for Science, Technology, and Innovations (MCTI). The CATERETÊ beamline staff is acknowledged for assistance during the experiments.This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). F.B.P. and Y.X. acknowledge Financiadora de Estudos e Projetos (FINEP), Fundação Carlos Chagas Filho de Amparo à Pesquisa do Estado do Rio de Janeiro (FAPERJ), and Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) for financial support. The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. The DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

MPM modeling
Mechanochemistry
PET upcycling
Raman microscopy
SAXS
depolymerization
reaction environment
spatially resolved spectroscopy

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10.1016/j.chempr.2025.102754

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title = "Spatially resolved reaction environments in mechanochemical upcycling of polymers",

abstract = "Mechanochemical processing is an attractive and scalable approach for the upcycling of polymers. The complex and dynamic environment in ball milling, however, makes gaining insight into the physicochemical nature of the collisions driving mechanochemistry challenging, which, in turn, hampers the optimization of these processes. We used controlled single impacts followed by multiple spatially resolved analytical methods (focused ion beam microscopy, Raman spectro-microscopy, and small-angle X-ray scattering) and material point method simulations to gain unprecedented information about mechanochemical depolymerization of poly(ethylene terephthalate). These measurements highlight the contributions of plastic deformation, amorphization, and depolymerization during the transfer of kinetic energy in collisions relevant to ball mills and will enable reactor models based on fundamental kinetics.",

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doi = "10.1016/j.chempr.2025.102754",

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AU - Gołąbek, Kinga

AU - Chang, Yuchen

AU - Mellinger, Lauren R.

AU - Rodrigues, Mariana V.

AU - de Souza Coutinho Nogueira, Cauê

AU - Passos, Fabio B.

AU - Xing, Yutao

AU - Ribeiro Passos, Aline

AU - Saffarini, Mohammed H.

AU - Isner, Austin B.

AU - Sholl, David S.

AU - Sievers, Carsten

PY - 2026/1/15

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N2 - Mechanochemical processing is an attractive and scalable approach for the upcycling of polymers. The complex and dynamic environment in ball milling, however, makes gaining insight into the physicochemical nature of the collisions driving mechanochemistry challenging, which, in turn, hampers the optimization of these processes. We used controlled single impacts followed by multiple spatially resolved analytical methods (focused ion beam microscopy, Raman spectro-microscopy, and small-angle X-ray scattering) and material point method simulations to gain unprecedented information about mechanochemical depolymerization of poly(ethylene terephthalate). These measurements highlight the contributions of plastic deformation, amorphization, and depolymerization during the transfer of kinetic energy in collisions relevant to ball mills and will enable reactor models based on fundamental kinetics.

AB - Mechanochemical processing is an attractive and scalable approach for the upcycling of polymers. The complex and dynamic environment in ball milling, however, makes gaining insight into the physicochemical nature of the collisions driving mechanochemistry challenging, which, in turn, hampers the optimization of these processes. We used controlled single impacts followed by multiple spatially resolved analytical methods (focused ion beam microscopy, Raman spectro-microscopy, and small-angle X-ray scattering) and material point method simulations to gain unprecedented information about mechanochemical depolymerization of poly(ethylene terephthalate). These measurements highlight the contributions of plastic deformation, amorphization, and depolymerization during the transfer of kinetic energy in collisions relevant to ball mills and will enable reactor models based on fundamental kinetics.

KW - MPM modeling

KW - Mechanochemistry

KW - PET upcycling

KW - Raman microscopy

KW - SAXS

KW - depolymerization

KW - reaction environment

KW - spatially resolved spectroscopy

UR - https://www.scopus.com/pages/publications/105025057465

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DO - 10.1016/j.chempr.2025.102754

M3 - Article

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SN - 2451-9308

VL - 12

JO - Chem

JF - Chem

IS - 1

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ER -

Spatially resolved reaction environments in mechanochemical upcycling of polymers

Abstract

Funding

Keywords

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