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Regulation of the Inevitable Water-Responsivity of Silk Fibroin Biopolymer by Polar Amino Acid Activation

Authors
 Woojin Choi  ;  Taesuk Jun  ;  Milae Lee  ;  Kyungtae Park  ;  Moonhyun Choi  ;  Sungwon Jung  ;  Jae-Kook Cha  ;  Jae-Sung Kwon  ;  Youngho Jin  ;  Sangmin Lee  ;  Du Yeol Ryu  ;  Jinkee Hong 
Citation
 ACS NANO, Vol.16(10) : 17274-17288, 2022-10 
Journal Title
ACS NANO
ISSN
 1936-0851 
Issue Date
2022-10
MeSH
Amino Acids ; Animals ; Bombyx* / chemistry ; Fibroins* / chemistry ; Humans ; Serine ; Silk / chemistry ; Swine ; Tissue Adhesives* ; Water / chemistry
Keywords
amino acid ; hydration-adaptive crystallization ; silk fibroin ; tissue adhesive ; water diffusion
Abstract
In nature, water is vital for maintaining homeostasis. Particularly, organisms (e.g., plant leaf, bird feather) exploit water fluidics for motions. Hydration-adaptive crystallization is the representative water-responsive actuation of biopolymers. This crystallization has inspired the development of intelligent human-robot interfaces. At the same time, it hinders the consistent adhesion of tissue adhesive. As hydration-adaptive crystallization is inevitable, the on-demand control of crystallization is desirable in the innovative biopolymeric biomedical systems. To this end, this study developed an amino acid-based technology to artificially up- or down-regulate the inevitable crystallization of silk fibroin. A case II diffusion model was constructed, and it revealed that the activity of polar amino acid is related to crystallization kinetics. Furthermore, the water dynamics study suggested that active amino acid stabilizes crystallization-triggering water molecules. As a proof-of-concept, we verified that a 30% increase in the activity of serine resulted in a 50% decrease in the crystallization rate. Furthermore, the active amino acid-based suppression of hydration-adaptive crystallization enabled the silk fibroin to keep its robust adhesion (approximately 160 kJ m-3) by reducing the water-induced loss of adhesive force. The proposed silk fibroin was demonstrated as a stable tissue adhesive applied on ex vivo porcine mandible tissue. This amino acid-based regulation of hydration-adaptive crystallization will pioneer next-generation biopolymer-based healthcare.
Full Text
https://pubs.acs.org/doi/10.1021/acsnano.2c07971
DOI
10.1021/acsnano.2c07971
Appears in Collections:
2. College of Dentistry (치과대학) > Dept. of Dental Biomaterials and Bioengineering (치과생체재료공학교실) > 1. Journal Papers
2. College of Dentistry (치과대학) > Dept. of Periodontics (치주과학교실) > 1. Journal Papers
Yonsei Authors
Kwon, Jae-Sung(권재성) ORCID logo https://orcid.org/0000-0001-9803-7730
Cha, Jae Kook(차재국) ORCID logo https://orcid.org/0000-0001-6817-9834
URI
https://ir.ymlib.yonsei.ac.kr/handle/22282913/192153
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