Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields

Sungjin Kim; Catherine Biju; Menisha S. Karunarathna; Niya Y. Grimes; Nadim S. Hmeidat; July Reyes-Zacarias; Shradha Agarwal; Md Anisur Rahman; Dustin B. Gilmer; Brett G. Compton; Steve E. Bullock; Tomonori Saito; Corson L. Cramer

doi:10.1016/j.cej.2024.156585

Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields

Sungjin Kim, Catherine Biju, Menisha S. Karunarathna, Niya Y. Grimes, Nadim S. Hmeidat, July Reyes-Zacarias, Shradha Agarwal, Md Anisur Rahman, Dustin B. Gilmer, Brett G. Compton, Steve E. Bullock, Tomonori Saito, Corson L. Cramer

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

Abstract

Control of preceramic polymer crosslinking for UV-curable processing is essential for fine 3D printing with high ceramic conversion for sustainable polymer-derived ceramics (PDC) engineering. While various factors influencing ceramic yield have been studied, the systematic exploration of the relationship between crosslinking and ceramic yield, especially when crosslinking increases volatile elements, remains open for further investigation. This study addresses this gap by utilizing vat photopolymerization (VP) additive manufacturing (AM) as a versatile platform for controlling preceramic crosslinking and ceramic yield. By rationally designing and tuning the photochemical crosslinking through digital light processing (DLP), we demonstrate that the ceramic yield can be enhanced from 64% to over 86%, even with added volatile elements. We reveal that the post-pyrolysis ceramic yield can be closely correlated with the pre-pyrolysis crosslinking of the preceramic network represented by its stiffness. This correlation thereby suggests a fast, energy-efficient, non-destructive methodology to predict and improve ceramic yield. Combined with these findings, our one-pot thiol-ene hybridization of polycarbosilane and polycarbosiloxane via DLP offers an exemplary method to generate hybrid preceramic polymers with tailored material properties toward target applications, and potentially even higher ceramic yields. This study thus contributes to achieving better resource- and energy-efficient preceramic polymer and PDC processing routes toward sustainable, advanced organic–inorganic materials manufacturing.

Original language	English
Article number	156585
Journal	Chemical Engineering Journal
Volume	499
DOIs	https://doi.org/10.1016/j.cej.2024.156585
State	Published - Nov 1 2024

Funding

This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy at Oak Ridge National Laboratory, and this material is based upon work supported by the state of Tennessee through the University of Tennessee\u2019s UT-Oak Ridge Innovation Institute (UT-ORII) Science Alliance Support for Affiliated Research Teams Program (StART Program). The first author acknowledges the startup funding from the Department of Chemical and Biological Engineering of the University of New Mexico . The first author also thanks Desarae J. Goldsby for training him on the Admatec 3D printer and equipment maintenance. This manuscript has been authored by UT-Battelle LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://energy.gov/downloads/doe-public-access-plan).

Keywords

Ceramic yield
Crosslinking
Digital light processing
Polymer-derived ceramics
Preceramic polymer
Sustainable manufacturing

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.cej.2024.156585

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Kim, S., Biju, C., Karunarathna, M. S., Grimes, N. Y., Hmeidat, N. S., Reyes-Zacarias, J., Agarwal, S., Anisur Rahman, M., Gilmer, D. B., Compton, B. G., Bullock, S. E., Saito, T., & Cramer, C. L. (2024). Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields. Chemical Engineering Journal, 499, Article 156585. https://doi.org/10.1016/j.cej.2024.156585

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title = "Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields",

abstract = "Control of preceramic polymer crosslinking for UV-curable processing is essential for fine 3D printing with high ceramic conversion for sustainable polymer-derived ceramics (PDC) engineering. While various factors influencing ceramic yield have been studied, the systematic exploration of the relationship between crosslinking and ceramic yield, especially when crosslinking increases volatile elements, remains open for further investigation. This study addresses this gap by utilizing vat photopolymerization (VP) additive manufacturing (AM) as a versatile platform for controlling preceramic crosslinking and ceramic yield. By rationally designing and tuning the photochemical crosslinking through digital light processing (DLP), we demonstrate that the ceramic yield can be enhanced from 64% to over 86%, even with added volatile elements. We reveal that the post-pyrolysis ceramic yield can be closely correlated with the pre-pyrolysis crosslinking of the preceramic network represented by its stiffness. This correlation thereby suggests a fast, energy-efficient, non-destructive methodology to predict and improve ceramic yield. Combined with these findings, our one-pot thiol-ene hybridization of polycarbosilane and polycarbosiloxane via DLP offers an exemplary method to generate hybrid preceramic polymers with tailored material properties toward target applications, and potentially even higher ceramic yields. This study thus contributes to achieving better resource- and energy-efficient preceramic polymer and PDC processing routes toward sustainable, advanced organic–inorganic materials manufacturing.",

keywords = "Ceramic yield, Crosslinking, Digital light processing, Polymer-derived ceramics, Preceramic polymer, Sustainable manufacturing",

author = "Sungjin Kim and Catherine Biju and Karunarathna, {Menisha S.} and Grimes, {Niya Y.} and Hmeidat, {Nadim S.} and July Reyes-Zacarias and Shradha Agarwal and {Anisur Rahman}, Md and Gilmer, {Dustin B.} and Compton, {Brett G.} and Bullock, {Steve E.} and Tomonori Saito and Cramer, {Corson L.}",

note = "Publisher Copyright: {\textcopyright} 2024",

year = "2024",

month = nov,

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doi = "10.1016/j.cej.2024.156585",

language = "English",

volume = "499",

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Kim, S, Biju, C, Karunarathna, MS, Grimes, NY, Hmeidat, NS, Reyes-Zacarias, J, Agarwal, S, Anisur Rahman, M, Gilmer, DB, Compton, BG, Bullock, SE , Saito, T & Cramer, CL 2024, 'Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields', Chemical Engineering Journal, vol. 499, 156585. https://doi.org/10.1016/j.cej.2024.156585

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AU - Kim, Sungjin

AU - Biju, Catherine

AU - Karunarathna, Menisha S.

AU - Grimes, Niya Y.

AU - Hmeidat, Nadim S.

AU - Reyes-Zacarias, July

AU - Agarwal, Shradha

AU - Anisur Rahman, Md

AU - Gilmer, Dustin B.

AU - Compton, Brett G.

AU - Bullock, Steve E.

AU - Saito, Tomonori

AU - Cramer, Corson L.

PY - 2024/11/1

Y1 - 2024/11/1

N2 - Control of preceramic polymer crosslinking for UV-curable processing is essential for fine 3D printing with high ceramic conversion for sustainable polymer-derived ceramics (PDC) engineering. While various factors influencing ceramic yield have been studied, the systematic exploration of the relationship between crosslinking and ceramic yield, especially when crosslinking increases volatile elements, remains open for further investigation. This study addresses this gap by utilizing vat photopolymerization (VP) additive manufacturing (AM) as a versatile platform for controlling preceramic crosslinking and ceramic yield. By rationally designing and tuning the photochemical crosslinking through digital light processing (DLP), we demonstrate that the ceramic yield can be enhanced from 64% to over 86%, even with added volatile elements. We reveal that the post-pyrolysis ceramic yield can be closely correlated with the pre-pyrolysis crosslinking of the preceramic network represented by its stiffness. This correlation thereby suggests a fast, energy-efficient, non-destructive methodology to predict and improve ceramic yield. Combined with these findings, our one-pot thiol-ene hybridization of polycarbosilane and polycarbosiloxane via DLP offers an exemplary method to generate hybrid preceramic polymers with tailored material properties toward target applications, and potentially even higher ceramic yields. This study thus contributes to achieving better resource- and energy-efficient preceramic polymer and PDC processing routes toward sustainable, advanced organic–inorganic materials manufacturing.

AB - Control of preceramic polymer crosslinking for UV-curable processing is essential for fine 3D printing with high ceramic conversion for sustainable polymer-derived ceramics (PDC) engineering. While various factors influencing ceramic yield have been studied, the systematic exploration of the relationship between crosslinking and ceramic yield, especially when crosslinking increases volatile elements, remains open for further investigation. This study addresses this gap by utilizing vat photopolymerization (VP) additive manufacturing (AM) as a versatile platform for controlling preceramic crosslinking and ceramic yield. By rationally designing and tuning the photochemical crosslinking through digital light processing (DLP), we demonstrate that the ceramic yield can be enhanced from 64% to over 86%, even with added volatile elements. We reveal that the post-pyrolysis ceramic yield can be closely correlated with the pre-pyrolysis crosslinking of the preceramic network represented by its stiffness. This correlation thereby suggests a fast, energy-efficient, non-destructive methodology to predict and improve ceramic yield. Combined with these findings, our one-pot thiol-ene hybridization of polycarbosilane and polycarbosiloxane via DLP offers an exemplary method to generate hybrid preceramic polymers with tailored material properties toward target applications, and potentially even higher ceramic yields. This study thus contributes to achieving better resource- and energy-efficient preceramic polymer and PDC processing routes toward sustainable, advanced organic–inorganic materials manufacturing.

KW - Ceramic yield

KW - Crosslinking

KW - Digital light processing

KW - Polymer-derived ceramics

KW - Preceramic polymer

KW - Sustainable manufacturing

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DO - 10.1016/j.cej.2024.156585

M3 - Article

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SN - 1385-8947

VL - 499

JO - Chemical Engineering Journal

JF - Chemical Engineering Journal

M1 - 156585

ER -

Tuning crosslinking of hybrid preceramic polymers in vat photopolymerization toward controlled ceramic Yields

Abstract

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Keywords

UN SDGs

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