Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect

Abstract Colloidal properties of nanoparticles are intricately linked to their morphology. Traditionally, achieving high-concentration dispersions of two-dimensional (2D) nanosheets has proven challenging as they tend to agglomerate or re-stack under increased surface contact and Van der Waals attra...

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Main Authors: Zhiyuan Xiong, Luyan Shen, Jin Long, Xiao Li, Ke Zhou, Gyeong Min Choi, Kangtai Ou, GuiYan Yang, Weichun Ma, Heon Sang Lee, Youyi Sun, Dan Li
Format: Article
Language:English
Published: Nature Portfolio 2024-12-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55131-y
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author Zhiyuan Xiong
Luyan Shen
Jin Long
Xiao Li
Ke Zhou
Gyeong Min Choi
Kangtai Ou
GuiYan Yang
Weichun Ma
Heon Sang Lee
Youyi Sun
Dan Li
author_facet Zhiyuan Xiong
Luyan Shen
Jin Long
Xiao Li
Ke Zhou
Gyeong Min Choi
Kangtai Ou
GuiYan Yang
Weichun Ma
Heon Sang Lee
Youyi Sun
Dan Li
author_sort Zhiyuan Xiong
collection DOAJ
description Abstract Colloidal properties of nanoparticles are intricately linked to their morphology. Traditionally, achieving high-concentration dispersions of two-dimensional (2D) nanosheets has proven challenging as they tend to agglomerate or re-stack under increased surface contact and Van der Waals attraction. Here, we unveil an excluded volume effect enabled by 2D morphology, which can be coupled with electrostatic repulsion to synthesize high-concentration aqueous graphene dispersions. To achieve this, we designed a sequential process involving edge oxidation, bubble expansion and mechanical shearing, through which graphite flakes were exfoliated into aqueous dispersions with ~94.5 wt.% yield of few-layer graphene, high concentration exceeding 100 mg mL-1, long-term stability over ~550 days, and large-scale wet processability. Structural analysis and theoretical modeling suggested that the 2D morphology of the resultant graphene nanosheets facilitates inter-sheet repulsive excluded volume interactions, leading to a fractal jammed network structure composed of nanosheets and tactoids to prevent their agglomeration. This effect was further leveraged in a continuous stirred tank reactor for the pilot-scale production of concentrated graphene dispersions. Our study unveils the role of excluded volume effect in stabilizing 2D-material colloids for industrial production and processing.
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spelling doaj-art-2f9b602e6a1c41f787cd45621b506a7e2025-01-05T12:34:57ZengNature PortfolioNature Communications2041-17232024-12-0115111110.1038/s41467-024-55131-yUltrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effectZhiyuan Xiong0Luyan Shen1Jin Long2Xiao Li3Ke Zhou4Gyeong Min Choi5Kangtai Ou6GuiYan Yang7Weichun Ma8Heon Sang Lee9Youyi Sun10Dan Li11School of Materials Science and Technology, North University of ChinaSchool of Materials Science and Technology, North University of ChinaSchool of Light Industry and Engineering, South China University of TechnologyDepartment of Environmental Science and Engineering, Fudan UniversityCollege of Energy, Soochow Institute for Energy and Materials InnovationS (SIEMIS), Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow UniversityDepartment of Chemical Engineering (BK-21 Four Graduate Program), Dong-A UniversitySchool of Light Industry and Engineering, South China University of TechnologySchool of Materials Science and Technology, North University of ChinaDepartment of Environmental Science and Engineering, Fudan UniversityDepartment of Chemical Engineering (BK-21 Four Graduate Program), Dong-A UniversitySchool of Materials Science and Technology, North University of ChinaDepartment of Chemical Engineering, The University of Melbourne, ParkvilleAbstract Colloidal properties of nanoparticles are intricately linked to their morphology. Traditionally, achieving high-concentration dispersions of two-dimensional (2D) nanosheets has proven challenging as they tend to agglomerate or re-stack under increased surface contact and Van der Waals attraction. Here, we unveil an excluded volume effect enabled by 2D morphology, which can be coupled with electrostatic repulsion to synthesize high-concentration aqueous graphene dispersions. To achieve this, we designed a sequential process involving edge oxidation, bubble expansion and mechanical shearing, through which graphite flakes were exfoliated into aqueous dispersions with ~94.5 wt.% yield of few-layer graphene, high concentration exceeding 100 mg mL-1, long-term stability over ~550 days, and large-scale wet processability. Structural analysis and theoretical modeling suggested that the 2D morphology of the resultant graphene nanosheets facilitates inter-sheet repulsive excluded volume interactions, leading to a fractal jammed network structure composed of nanosheets and tactoids to prevent their agglomeration. This effect was further leveraged in a continuous stirred tank reactor for the pilot-scale production of concentrated graphene dispersions. Our study unveils the role of excluded volume effect in stabilizing 2D-material colloids for industrial production and processing.https://doi.org/10.1038/s41467-024-55131-y
spellingShingle Zhiyuan Xiong
Luyan Shen
Jin Long
Xiao Li
Ke Zhou
Gyeong Min Choi
Kangtai Ou
GuiYan Yang
Weichun Ma
Heon Sang Lee
Youyi Sun
Dan Li
Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
Nature Communications
title Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
title_full Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
title_fullStr Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
title_full_unstemmed Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
title_short Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect
title_sort ultrahigh concentration exfoliation and aqueous dispersion of few layer graphene by excluded volume effect
url https://doi.org/10.1038/s41467-024-55131-y
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