Muhammad Prayogie Aulia, Keizo Nakagawa, Tooru Kitagawa, Ralph Rolly Gonzales, Yasunao Okamoto, Atsushi Matsuoka, Eiji Kamio, Tomohisa Yoshioka, Sri Mulyati, Nasrul Arahman, Hideto Matsuyama
Fluorine-free bio-based membrane modification offers a sustainable pathway to developing hydrophobic membranes for high-performance oil dehydration. Herein, a hydrophobic biopolymer derived from chitin was incorporated into a polyacrylonitrile (PAN) spinning solution to fabricate modified electrospun nanofiber membranes without using fluorinated compounds. The incorporation of the biopolymer effectively transformed the intrinsically hydrophilic PAN nanofiber membrane into a hydrophobic surface, increasing the water contact angle from approximately 40° for pristine PAN to approximately 120° at a 4 wt% biopolymer loading. This modification also altered fiber stiffness, surface roughness, and nanofibrous morphology, thereby improving oil permeation and water rejection. FTIR and XPS analyses confirmed the successful incorporation of the hydrophobic biopolymer through physical blending without detectable chemical reaction. At the same time, molecular dynamics simulations revealed good compatibility and homogeneous dispersion within the PAN matrix. Benefiting from the interconnected nanofiber structure and enhanced hydrophobicity, the modified PAN membrane exhibited excellent oil dehydration performance, achieving a toluene permeance of approximately 15,000 LMH/bar and oil purity exceeding 99.8%. Moreover, the membrane retained more than 90% of its initial permeance and maintained stable wettability after 10 repeated separation cycles, demonstrating strong operational durability. This study highlights the potential of hydrophobic biopolymers as environmentally benign modifiers for the design of fluorine-free nanofiber membranes for efficient and sustainable oil dehydration. © 2026 Elsevier B.V.
Department of Chemical Science and Engineering, Kobe University, 1-1 Rokkodai, Nada, Kobe, 657-8501, Japan; Research Center for Membrane and Film Technology, Kobe University, 1-1 Rokkodai, Nada, Kobe, 657-8501, Japan; of Science, Technology and Innovation, Kobe University, 1-1 Rokkodai, Nada, Kobe, 657-8501, Japan; New Zealand Institute for Bioeconomy Science, Titokorangi Drive, Private Bag 3020, Rotorua, 3010, New Zealand; Department of Chemical Engineering, Universitas Syiah Kuala, Banda Aceh, 23111, Indonesia
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