Enhanced Catalytic Dechlorination of Polyvinyl Chloride (PVC) and H2 Production Enabled by Synergistic Gaδ+/Ga0 Active Sites in Liquid Metal Particles.
5 affiliations
- 1Department of Chemistry, Kentucky State University.Frankfort, Kentucky40601, United States.
- 2Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee37831, United States.
- 3Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee37831, United States.
- 4Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee37831, United States.
- 5Chemical and Biomolecular Engineering Department, Vanderbilt University, Nashville, Tennessee37235, United States.
Abstract
Polyvinyl chloride (PVC) is ubiquitous yet challenging to recycle due to its tendency to thermally decompose above 250 °C, releasing toxic, corrosive chlorinated compounds, and its inability to melt. Here, we report a catalytic strategy for PVC upcycling at 160 °C using gallium liquid metal particles (Ga-LMP) featuring a dynamic Ga-GaOOH core-shell architecture. These catalysts enable concurrent dechlorination and hydrogen evolution, yielding up to 7% H2 (based on initial hydrogen atoms in PVC) along with a highly dechlorinated (>95%) carbonaceous solid and aqueous HCl. Mechanistic investigations combining X-ray photoelectron spectroscopy, infrared spectroscopy, solid-state NMR, inelastic neutron scattering, and ab initio molecular dynamics reveal a synergistic interplay between Gaδ+ sites in the GaOOH shell and metallic Ga0 in the core. Cationic Ga initiates C-Cl bond activation and HCl formation, while progressive reduction of the shell exposes Ga0 sites that promote C-H activation and H2 evolution. Control experiments with a Ga salt and bulk Ga liquid metal confirmed that neither oxidation state alone can achieve both transformations efficiently. This work establishes a dynamic dual-site paradigm for liquid metal catalysis, in which the in situ evolution and coexistence of oxidized and metallic species enable sequential and cooperative bond activation pathways. These findings provide a general design principle for novel liquid metal catalysts that target challenging polymer transformations under mild conditions.
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BibTeX
@article{zingg2026enhanced,
title = {{Enhanced Catalytic Dechlorination of Polyvinyl Chloride (PVC) and H2 Production Enabled by Synergistic Gaδ+/Ga0 Active Sites in Liquid Metal Particles.}},
author = {Benjamin H Crockett Zingg and Nabihan B Abdul Rahman and Nishu Devi and Anya Zornes and Joshua T Damron and Ernesto C Zuleta S and Yan-Ru Lin and José David Arregui-Mena and Chang Liu and Murillo Longo Martins and Shukai Yao and Mo Li and De-En Jiang and Harry M Meyer and Zili Wu and Felipe Polo-Garzon},
journal = {Journal of the American Chemical Society},
year = {2026},
month = sep,
doi = {10.1021/jacs.6c09418},
url = {https://europepmc.org/article/MED/42915535},
note = {CC BY},
}
RIS
TY - JOUR
TI - Enhanced Catalytic Dechlorination of Polyvinyl Chloride (PVC) and H2 Production Enabled by Synergistic Gaδ+/Ga0 Active Sites in Liquid Metal Particles.
AU - Benjamin H Crockett Zingg
AU - Nabihan B Abdul Rahman
AU - Nishu Devi
AU - Anya Zornes
AU - Joshua T Damron
AU - Ernesto C Zuleta S
AU - Yan-Ru Lin
AU - José David Arregui-Mena
AU - Chang Liu
AU - Murillo Longo Martins
AU - Shukai Yao
AU - Mo Li
AU - De-En Jiang
AU - Harry M Meyer
AU - Zili Wu
AU - Felipe Polo-Garzon
PY - 2026
DA - 2026/09/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c09418
UR - https://europepmc.org/article/MED/42915535
AB - Polyvinyl chloride (PVC) is ubiquitous yet challenging to recycle due to its tendency to thermally decompose above 250 °C, releasing toxic, corrosive chlorinated compounds, and its inability to melt. Here, we report a catalytic strategy for PVC upcycling at 160 °C using gallium liquid metal particles (Ga-LMP) featuring a dynamic Ga-GaOOH core-shell architecture. These catalysts enable concurrent dechlorination and hydrogen evolution, yielding up to 7% H2 (based on initial hydrogen atoms in PVC) along with a highly dechlorinated (>95%) carbonaceous solid and aqueous HCl. Mechanistic investigations combining X-ray photoelectron spectroscopy, infrared spectroscopy, solid-state NMR, inelastic neutron scattering, and ab initio molecular dynamics reveal a synergistic interplay between Gaδ+ sites in the GaOOH shell and metallic Ga0 in the core. Cationic Ga initiates C-Cl bond activation and HCl formation, while progressive reduction of the shell exposes Ga0 sites that promote C-H activation and H2 evolution. Control experiments with a Ga salt and bulk Ga liquid metal confirmed that neither oxidation state alone can achieve both transformations efficiently. This work establishes a dynamic dual-site paradigm for liquid metal catalysis, in which the in situ evolution and coexistence of oxidized and metallic species enable sequential and cooperative bond activation pathways. These findings provide a general design principle for novel liquid metal catalysts that target challenging polymer transformations under mild conditions.
SN - 0002-7863
SN - 1520-5126
ER -