Abstract
L−3,4-dihydroxyphenylalanine is an important molecule in the adhesion of mussels, and as an oxidative precursor of natural melanin, it plays an important role in living system. Here, we investigate the effect of the molecular chirality of 3,4-dihydroxyphenylalanine on the properties of the self-assembled films by tyrosinase-induced oxidative polymerization. The kinetics and morphology of pure enantiomers are completely altered upon their co-assembly, allowing the fabrication of layer-to-layer stacked nanostructures and films with improved structural and thermal stability. The different molecular arrangements and self-assembly mechanisms of the L+D-racemic mixtures, whose oxidation products have increased binding energy, resulting in stronger intermolecular forces, which significantly increases the elastic modulus. This study provides a simple pathway for the fabrication of biomimetic polymeric materials with enhanced physicochemical properties by controlling the chirality of monomers.
Original language | American English |
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Article number | 3054 |
Journal | Nature Communications |
Volume | 14 |
Issue number | 1 |
DOIs | |
State | Published - Dec 2023 |
Bibliographical note
Funding Information:This work was supported by the Natural Science Foundation of China (Nos. 22278306 (Y.W. from Tianjin University), 22078239 (W.Q.), and 22278314 (W.Q.)), the National Key Research and Development Program of China (No. 2019YFE0106900 (R.S.)), the National Administration of Traditional Chinese Medicine (ZYYCXTD-D-202002 (Y.W. from Tianjin University of Traditional Chinese Medicine)), the Independent Innovation Funding of Tianjin University (No. 2023XJD-0067 (Y.W. from Tianjin University)), and the State Key Laboratory of Chemical Engineering (SKL-ChE-21T03 (Y.W. from Tianjin University), and SKL-ChE-22T05 (W.Q.)). The characterization results were supported by Beijing Zhongkebaice Technology Service Co., Ltd (www.zkbaice.cn). The authors thank Prof. Zhonghua Wu and Dr. Guang Mo of BSRF for assistance with the SAXS measurement, thank Dr. Yu Chen of BSRF for the GIWAXS measurement, thank Xiao Liu and Yiming Zheng from TJU and Haipeng Liu from Shiyanjia Lab (www.shiyanjia.com) for the SPR analysis and tensile and bonding strength tests and friction tests and thank Dr. Kongying Zhu at the Center for Nuclear Magnetic Analysis, Tianjin University for the solid-state NMR guidance.
Funding Information:
This work was supported by the Natural Science Foundation of China (Nos. 22278306 (Y.W. from Tianjin University), 22078239 (W.Q.), and 22278314 (W.Q.)), the National Key Research and Development Program of China (No. 2019YFE0106900 (R.S.)), the National Administration of Traditional Chinese Medicine (ZYYCXTD-D-202002 (Y.W. from Tianjin University of Traditional Chinese Medicine)), the Independent Innovation Funding of Tianjin University (No. 2023XJD-0067 (Y.W. from Tianjin University)), and the State Key Laboratory of Chemical Engineering (SKL-ChE-21T03 (Y.W. from Tianjin University), and SKL-ChE-22T05 (W.Q.)). The characterization results were supported by Beijing Zhongkebaice Technology Service Co., Ltd ( www.zkbaice.cn ). The authors thank Prof. Zhonghua Wu and Dr. Guang Mo of BSRF for assistance with the SAXS measurement, thank Dr. Yu Chen of BSRF for the GIWAXS measurement, thank Xiao Liu and Yiming Zheng from TJU and Haipeng Liu from Shiyanjia Lab ( www.shiyanjia.com ) for the SPR analysis and tensile and bonding strength tests and friction tests and thank Dr. Kongying Zhu at the Center for Nuclear Magnetic Analysis, Tianjin University for the solid-state NMR guidance.
Publisher Copyright:
© 2023, The Author(s).