Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing

Ali Kamali; Joshua M. Little; Song Luo; Amy Chen; Akash Warty; Antara Bhowmick; Jorge Moncada; Evan P. Jahrman; Brandon C. Vance; Jong K. Keum; Taylor J. Woehl; Po Yen Chen; Dionisios G. Vlachos; Dongxia Liu

doi:10.1016/j.checat.2025.101459

Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing

Ali Kamali
, Joshua M. Little
, Song Luo
, Amy Chen
, Akash Warty
, Antara Bhowmick
, Jorge Moncada
, Evan P. Jahrman
, Brandon C. Vance
, Jong K. Keum
, Taylor J. Woehl
, Po Yen Chen
, Dionisios G. Vlachos
, Dongxia Liu

Functional Hybrid Nanomaterials

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

2 Scopus citations

Abstract

The hydrogenolysis of plastics is limited by active-site inaccessibility and inefficient mass transport of bulky polymer chains. To overcome these challenges, this work developed two-dimensional MXene-supported Ru (Ru@MXene) catalysts. Lyophilization of a solution containing dispersed MXene sheets and Ru precursors enabled the confinement of Ru species within the MXene interlayers, which act as pillars to expand the interlayer spacing. Building on this, a silica-pillared MXene-supported Ru (Ru@P-MXene) with even larger interlayer spacing exhibited a reaction rate of 914.9 g_C5–C35 g_Ru⁻¹ h⁻¹ for the hydrogenolysis of low-density polyethylene (LDPE) into valuable liquid chemicals (e.g., C₅–C₃₅). A comparison of product yields between Ru@P-MXene and Ru@MXene suggests that elongated Ru particles confined within the MXene support expose their side facets for the reaction. This work demonstrates a new application of MXene in thermochemical catalysis, offering a solution to the challenges of active-site accessibility, mass transport, and reaction confinement in chemical plastic upcycling.

Original language	English
Article number	101459
Journal	Chem Catalysis
Volume	5
Issue number	9
DOIs	https://doi.org/10.1016/j.checat.2025.101459
State	Published - Sep 18 2025

Funding

This work was supported as part of the Center for Plastics Innovation, an Energy Frontier Research Center funded by the Basic Energy Sciences program of US Department of Energy (DOE) Office of Science under grant no. DE-SC0021166 . This research used beamlines 6-BM and 8-ID of the National Synchrotron Light Source II, a US DOE Office of Science User Facility operated by Brookhaven National Laboratory under contract no. DE-SC0012704 . This work used the ARM200F transmission electron microscope at the US Army Combat Capabilities Development Command Army Research Laboratory under ARL Cooperative Research and Development Agreement no. CRADA 14-052-22 . This research also used the resources of the Center for Nanophase Materials Sciences (CNMS) and the Spallation Neutron Source (SNS), both US DOE Office of Science User Facilities operated by Oak Ridge National Laboratory.

Keywords

2D materials
MXene
Ru/MXene
SDG7: Affordable and clean energy
SDG9: Industry, innovation, and infrastructure
confinement
hydrogenolysis
mass-transport limitation
mesoporous MXene
plastic waste
polyolefin
ruthenium

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10.1016/j.checat.2025.101459

Cite this

Kamali, A., Little, J. M., Luo, S., Chen, A., Warty, A., Bhowmick, A., Moncada, J., Jahrman, E. P., Vance, B. C., Keum, J. K., Woehl, T. J., Chen, P. Y., Vlachos, D. G., & Liu, D. (2025). Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing. Chem Catalysis, 5(9), Article 101459. https://doi.org/10.1016/j.checat.2025.101459

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title = "Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing",

abstract = "The hydrogenolysis of plastics is limited by active-site inaccessibility and inefficient mass transport of bulky polymer chains. To overcome these challenges, this work developed two-dimensional MXene-supported Ru (Ru@MXene) catalysts. Lyophilization of a solution containing dispersed MXene sheets and Ru precursors enabled the confinement of Ru species within the MXene interlayers, which act as pillars to expand the interlayer spacing. Building on this, a silica-pillared MXene-supported Ru (Ru@P-MXene) with even larger interlayer spacing exhibited a reaction rate of 914.9 gC5–C35 gRu−1 h−1 for the hydrogenolysis of low-density polyethylene (LDPE) into valuable liquid chemicals (e.g., C5–C35). A comparison of product yields between Ru@P-MXene and Ru@MXene suggests that elongated Ru particles confined within the MXene support expose their side facets for the reaction. This work demonstrates a new application of MXene in thermochemical catalysis, offering a solution to the challenges of active-site accessibility, mass transport, and reaction confinement in chemical plastic upcycling.",

keywords = "2D materials, MXene, Ru/MXene, SDG7: Affordable and clean energy, SDG9: Industry, innovation, and infrastructure, confinement, hydrogenolysis, mass-transport limitation, mesoporous MXene, plastic waste, polyolefin, ruthenium",

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AU - Kamali, Ali

AU - Little, Joshua M.

AU - Luo, Song

AU - Chen, Amy

AU - Warty, Akash

AU - Bhowmick, Antara

AU - Moncada, Jorge

AU - Jahrman, Evan P.

AU - Vance, Brandon C.

AU - Keum, Jong K.

AU - Woehl, Taylor J.

AU - Chen, Po Yen

AU - Vlachos, Dionisios G.

AU - Liu, Dongxia

PY - 2025/9/18

Y1 - 2025/9/18

N2 - The hydrogenolysis of plastics is limited by active-site inaccessibility and inefficient mass transport of bulky polymer chains. To overcome these challenges, this work developed two-dimensional MXene-supported Ru (Ru@MXene) catalysts. Lyophilization of a solution containing dispersed MXene sheets and Ru precursors enabled the confinement of Ru species within the MXene interlayers, which act as pillars to expand the interlayer spacing. Building on this, a silica-pillared MXene-supported Ru (Ru@P-MXene) with even larger interlayer spacing exhibited a reaction rate of 914.9 gC5–C35 gRu−1 h−1 for the hydrogenolysis of low-density polyethylene (LDPE) into valuable liquid chemicals (e.g., C5–C35). A comparison of product yields between Ru@P-MXene and Ru@MXene suggests that elongated Ru particles confined within the MXene support expose their side facets for the reaction. This work demonstrates a new application of MXene in thermochemical catalysis, offering a solution to the challenges of active-site accessibility, mass transport, and reaction confinement in chemical plastic upcycling.

AB - The hydrogenolysis of plastics is limited by active-site inaccessibility and inefficient mass transport of bulky polymer chains. To overcome these challenges, this work developed two-dimensional MXene-supported Ru (Ru@MXene) catalysts. Lyophilization of a solution containing dispersed MXene sheets and Ru precursors enabled the confinement of Ru species within the MXene interlayers, which act as pillars to expand the interlayer spacing. Building on this, a silica-pillared MXene-supported Ru (Ru@P-MXene) with even larger interlayer spacing exhibited a reaction rate of 914.9 gC5–C35 gRu−1 h−1 for the hydrogenolysis of low-density polyethylene (LDPE) into valuable liquid chemicals (e.g., C5–C35). A comparison of product yields between Ru@P-MXene and Ru@MXene suggests that elongated Ru particles confined within the MXene support expose their side facets for the reaction. This work demonstrates a new application of MXene in thermochemical catalysis, offering a solution to the challenges of active-site accessibility, mass transport, and reaction confinement in chemical plastic upcycling.

KW - 2D materials

KW - MXene

KW - Ru/MXene

KW - SDG7: Affordable and clean energy

KW - SDG9: Industry, innovation, and infrastructure

KW - confinement

KW - hydrogenolysis

KW - mass-transport limitation

KW - mesoporous MXene

KW - plastic waste

KW - polyolefin

KW - ruthenium

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DO - 10.1016/j.checat.2025.101459

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JO - Chem Catalysis

JF - Chem Catalysis

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ER -

Plastic-waste hydrogenolysis over two-dimensional MXene-supported ruthenium catalysts with tunable interlayer spacing

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