journal article·2024-10-23

Biorenewable Exfoliation of Electronic-Grade Printable Graphene Using Carboxylated Cellulose Nanocrystals

Janan Hui, Haoyang You, Anton Van Beek, Jinrui Zhang, Arash Elahi, Julia R. Downing, Lindsay E. Chaney, DoKyoung Lee, Elizabeth A. Ainsworth, Santanu Chaudhuri, Jennifer B. Dunn, Wei Chen, Stuart J. Rowan, Mark C. Hersam

ACS Applied Materials & Interfaces· Volume 16· Issue 42
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Abstract

The absence of scalable and environmentally sustainable methods for producing electronic-grade graphene nanoplatelets remains a barrier to the industrial-scale application of graphene in printed electronics and conductive composites. To address this unmet need, here we report the utilization of carboxylated cellulose nanocrystals (CNCs) extracted from the perennial tall grass Miscanthus × giganteus as a biorenewable dispersant for the aqueous liquid-phase exfoliation of few-layer graphene nanoplatelets. This CNC-based exfoliation procedure was optimized using a Bayesian machine learning model, resulting in a significant graphite-to-graphene conversion yield of 13.4% and a percolating graphene thin-film electrical conductivity of 3.4 × 10 4 S m –1 . The as-exfoliated graphene dispersions were directly formulated into an aerosol jet printing ink using cellulose-based additives to achieve high-resolution printing (∼20 μm line width). Life cycle assessment of this CNC-based exfoliation method showed substantial improvements for fossil fuel consumption, greenhouse gas emissions, and water consumption compared to incumbent liquid-phase exfoliation methods for electronic-grade graphene nanoplatelets. Mechanistically, potential mean force calculations from molecular dynamics simulations reveal that the high exfoliation yield can be traced back to the favorable surface interactions between CNCs and graphene. Ultimately, the use of biorenewable CNCs for liquid-phase exfoliation will accelerate the scalable and eco-friendly manufacturing of graphene for electronically conductive applications.
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Research context

OpenAlex topics: Graphene and Nanomaterials Applications · Electrohydrodynamics and Fluid Dynamics · Advanced Sensor and Energy Harvesting Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States

Department of Chemistry, University of Chicago, 5735 South Ellis Avenue, Chicago, Illinois 60637 United States

Department of Mechanical Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States

Department of Chemical and Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States

Department of Chemical Engineering, University of Illinois at Chicago, 929 West Taylor Street, Chicago, Illinois 60607, United States

Department of Materials Science and Engineering, Northwestern University, 2220 Campus Drive, Evanston, Illinois 60208, United States

Department of Crop Sciences, University of Illinois at Urbana−Champaign, 1102 South Goodwin Avenue, Urbana, Illinois 61801, United States

Global Change and Photosynthesis Research Unit, Agricultural Research Service (ARS), United States Department of Agriculture (USDA), Urbana, Illinois 61801, United States

Department of Civil, Materials, and Environmental Engineering, University of Illinois at Chicago, 842 West Taylor Street, Chicago, Illinois 60607, United States

Pritzker School of Molecular Engineering, University of Chicago, 5640 South Ellis Avenue, Chicago, Illinois 60637, United States

Chemical and Engineering Sciences, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439 United States

Department of Electrical and Computer Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States

Funding

National Institute of Standards and Technology · National Science Foundation

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