Citation: Wenqian He, Ya Di, Nan Jiang, Zunfeng Liu, Yongsheng Chen. Graphene-Oxide Seeds Nucleate Strong and Tough Hydrogel-Based Artificial Spider Silk[J]. Acta Physico-Chimica Sinica, ;2022, 38(9): 220405. doi: 10.3866/PKU.WHXB202204059 shu

Graphene-Oxide Seeds Nucleate Strong and Tough Hydrogel-Based Artificial Spider Silk

Wenqian He ¹ ,
Ya Di ² ,
Nan Jiang ² ,
Zunfeng Liu ^1,, ,
Yongsheng Chen ^1,,

1.
State Key Laboratory of Medicinal Chemical Biology, Key Laboratory of Functional Polymer Materials, College of Chemistry, Nankai University, Tianjin 300071, China
2.
Innovation Center of Hangyu Lifesaving Equipment, Wuhan 430000, China

Corresponding author: Zunfeng Liu, liuzunfeng@nankai.edu.cn Yongsheng Chen, yschen99@nankai.edu.cn
Received Date: 30 April 2022
Revised Date: 13 June 2022
Accepted Date: 15 June 2022
Available Online: 22 June 2022
Fund Project: the National Natural Science Foundation of China 52090034the National Natural Science Foundation of China 51973093the National Natural Science Foundation of China 51773094the National Key Research and Development Program of China 2019YFE0119600Frontiers Science Center for New Organic Matter, Nankai University 63181206

Natural spider silk is composed of spun spidroin protein containing beta-sheet crosslinking sites drawn from an S-shaped spinning duct. It exhibits an excellent combination of strength (1150 ± 200 MPa) and toughness (165 ± 30 MJ·m⁻³) that originates from its hierarchical structure, including crosslinking sites, highly aligned nano-aggregates, and a sheath-core structure. In this work, we prepared a hydrogel fiber that contains crosslinking sites, highly aligned nano-aggregates, and a sheath-core structure, by draw-spinning a bulk hydrogel composed of polyacrylic acid crosslinked with vinyl-functionalized silica nanoparticles (SNVs). The core-sheath structure was prepared by the water-evaporation-controlled self-assembly of the polyacrylic hydrogel, while nanometer-sized aggregates were formed by the self-assembly of polyacrylic acid chains. The addition of a tiny amount of graphene oxide (GO: 0.01%), a 2D nanomaterial, enhanced the mechanical properties of the fiber (breaking strength: 560 MPa; fracture toughness: 200 MJ·m⁻³; damping capacity: 94%). In addition, we investigated the factors responsible for the mechanical properties of the gel fibers, including fiber diameter, drying time in air, relative air humidity, and stretching speed. A higher breaking strength and a lower fracture strain was obtained by decreasing the fiber diameter, increasing the drying time, or increasing the stretching speed, while a lower fracture strain and higher breaking strength were obtained by increasing the relative air humidity. Polarized optical and SEM images revealed that the GO-seeded material is better aligned and contains smaller nano-aggregates, with GO seeding found to play a key role in the formation of nano-aggregates and polymer-chain alignment. The prepared fiber exhibited excellent mechanical properties compared to gel fibers prepared by other methods (e.g., electro-, wet, dry, and microfluidic spinning, as well as templating, and 3D printing, etc.). Repeated mechanical testing involving stretch-release cycles to 70% strain at 20% relative humidity revealed that the fibers have an energy-damping capacity of 93.6%, which exceeds that of natural spider silk and many types of artificial fiber. The relaxed stretched fiber recovered its initial length when exposed to 80% relative humidity, while the fiber recovered its initial mechanical properties when stored for 2 h at room temperature. A yarn composed of three hundred of the prepared gel fibers was shown to lift a 3 kg object without breaking; the prepared fiber was also shown to absorb dynamic energy and lower the impact force of a falling object.
- Functional fiber,
- Polymer composite,
- Biomimetic,
- Spinning,
- Nanomaterials,
- Graphene oxide,
- Damp capacity
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