Molecular tuning of DNA framework–programmed silicification by cationic silica cluster attachment
Abstract
The organizational complexity of biominerals has long fascinated scientists seeking to understand biological programming and implement new developments in biomimetic materials chemistry. Nonclassical crystallization pathways have been observed and analyzed in typical crystalline biominerals, such as calcium phosphate, calcium carbonate, and ferric oxide, involving the controlled attachment and reconfiguration of nanoparticles and clusters on organic templates. However, the understanding of templated amorphous silica mineralization remains limited, hindering the rational design of complex silica-based materials. Here, we report the finding of ultrastable and monodispersed cationic silica cluster (CSC) and their assembly using DNA nanostructures as programmable attachment templates. Cryo-EM imaging reveal that a typical CSC with a diameter of gyration of ~3.9 nm and an average molecular weight of ~8, 262 Da is characteristic of a branched hierarchical structure. We demonstrate high-fidelity silicification by tuning the composition and structure of CSC, providing a unified model of silicification by cluster attachment. Our findings pave the way toward the molecular tuning of pre- and postnucleation stages of sol–gel reactions and provide insights for the design of silica-based materials with controlled organization and functionality.
Article Details
Journal Info
Proceedings of the National Academy of Sciences
National Academy of Sciences
Authors (18)
Xinxin Jing
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine, Shanghai Jiao Tong University
Haozhi Wang
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study and National Center for Translational Medicine
Jianxiang Huang
Yingying Liu
Institute of Intelligent Machines, Hefei Institutes of Physical Science
Zimu Li
Jielin Chen
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine, Shanghai Jiao Tong University
Yiqun Xu
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine, Shanghai Jiao Tong University
Lingyun Li
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine, Shanghai Jiao Tong University
Yunxiao Lin
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study and National Center for Translational Medicine
Damiano Buratto
Institute of Quantitative Biology, College of Life Sciences, and Department of Physics, Zhejiang University
Qinglin Xia
Division of Physical Biology, Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Muchen Pan
Division of Physical Biology, Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Yue Wang
Mingqiang Li
State Key Laboratory of Synergistic Chem-Bio Synthesis, State Key Laboratory of Micro-Nano Engineering Science, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study, and National Center for Translational Medicine
Ruhong Zhou
Stephen Mann
Chunhai Fan
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine
Xiaoguo Liu
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study and National Center for Translational Medicine