Supramolecular Scale Hydrophilicity Regulation Enabling Efficient Dewatering and Assembly of Nanocellulose into Dense and Strong Bulk Materials as Sustainable Plastic Substitutes

J Jie Zhou Y Yifan Ma J Junqing Chen (Hubei Biomass‐Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials School of Resource and Environmental Sciences Wuhan University Wuhan 430079 China) Z Ziyan Cai (Hubei Biomass‐Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials School of Resource and Environmental Sciences Wuhan University Wuhan 430079 China) L Luhe Qi J Jinyi Cui (State Key Laboratory of Advanced Papermaking and Paper‐based Materials, School of Light Industry and Engineering South China University of Technology Guangzhou 510641 China) S Shilin Deng W Wengen Ouyang (Department of Engineering Mechanics, School of Civil Engineering, Wuhan University 3 , Wuhan, Hubei 430072,) Z Zhiqiang Fang (State Key Laboratory of Advanced Papermaking and Paper‐based Materials, School of Light Industry and Engineering South China University of Technology Guangzhou 510641 China) X Xueqing Qiu (Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry) C Chaoji Chen (Hubei Key Laboratory of Biomass Resource Chemistry and Environmental Biotechnology, Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, Hubei Engineering Center of Natural Polymers-based Medical Materials, School of Resource and Environmental Science, Wuhan University)

Abstract

Abstract Cellulose nanofibers (CNFs) are ideal building blocks for creating lightweight and strong bulk structural materials due to their unique supramolecular structure and exceptional mechanical properties within the crystalline regions. However, assembling CNFs into dense bulk structural materials with customizable shape and functionalities remains a great challenge, hindering their practical applications. Here, the dewatering issue of aqueous CNF dispersions is addressed by regulating supramolecular scale hydrophilicity using lactic acid, combined with hot‐press molding. This approach enables the fabrication of transparent CNF bulk structural materials with a density of up to 1.426 g cm −3 . The mechanical properties, including isotropic in‐plane tensile strength (75.5 ± 4.5 MPa), flexural strength (198 ± 20 MPa), and hardness (≈300 MPa), surpass most engineering plastics. Moreover, unlike conventional CNF based materials, the CNF bulk structural materials exhibit remarkable water stability and flame retardancy. These unique advantages open a new avenue to bottom‐up assembly of CNFs into high‐performance multifunctional eco‐friendly structural materials, dedicating to substitution of plastics and easing the consumption of petrochemical resources.

Article Details

Volume / Issue Vol. 37, Issue 9
Published March 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (11)

J

Jie Zhou

Y

Yifan Ma

J

Junqing Chen

Hubei Biomass‐Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials School of Resource and Environmental Sciences Wuhan University Wuhan 430079 China

Z

Ziyan Cai

Hubei Biomass‐Resource Chemistry and Environmental Biotechnology Key Laboratory, Hubei Provincial Engineering Research Center of Emerging Functional Coating Materials School of Resource and Environmental Sciences Wuhan University Wuhan 430079 China

L

Luhe Qi

J

Jinyi Cui

State Key Laboratory of Advanced Papermaking and Paper‐based Materials, School of Light Industry and Engineering South China University of Technology Guangzhou 510641 China

S

Shilin Deng

W

Wengen Ouyang

Department of Engineering Mechanics, School of Civil Engineering, Wuhan University 3 , Wuhan, Hubei 430072,

Z

Zhiqiang Fang

State Key Laboratory of Advanced Papermaking and Paper‐based Materials, School of Light Industry and Engineering South China University of Technology Guangzhou 510641 China

X

Xueqing Qiu

Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry

C

Chaoji Chen

Hubei Key Laboratory of Biomass Resource Chemistry and Environmental Biotechnology, Hubei International Scientific and Technological Cooperation Base of Sustainable Resource and Energy, Hubei Engineering Center of Natural Polymers-based Medical Materials, School of Resource and Environmental Science, Wuhan University