School of Chemistry and Chemical Engineering, Frontiers Science Centre for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China.
Center for Molecular Design and Biomimetics, The Biodesign Institute, School of Molecular Sciences, Arizona State University, Tempe, AZ, 85281, USA.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16693-16699. doi: 10.1002/anie.202106010. Epub 2021 Jun 18.
Long-range electrostatic interactions beyond biomolecular interaction interfaces have not been extensively studied due to the limitation in engineering electric double layers in physiological fluids. Here we find that long-range electrostatic interactions play an essential role in kinetic modulation of DNA hybridizations. Protein and gold nanoparticles with different charges are encapsulated in tetrahedral frameworks to exert diverse electrostatic effects on site-specifically tethered single DNA strands. Using this strategy, we have successfully modulated the hybridization kinetics in both bulk solution and single molecule level. Experimental and theoretical studies reveal that long-range Coulomb interactions are the key factor for hybridization rates. This work validates the important role of long-range electrostatic forces in nucleic acid-biomacromolecule complexes, which may encourage new strategies of gene regulation, antisense therapy, and nucleic acid detection.
由于在生理流体中构建电双层的技术限制，长程静电相互作用在生物分子相互作用界面之外的研究还不够广泛。在这里，我们发现长程静电相互作用在 DNA 杂交的动力学调节中起着至关重要的作用。具有不同电荷的蛋白质和金纳米粒子被包裹在四面体形框架中，以对特异性固定的单链 DNA 施加不同的静电效应。利用这种策略，我们成功地调节了在体相溶液和单分子水平上的杂交动力学。实验和理论研究表明，长程库仑相互作用是杂交速率的关键因素。这项工作验证了长程静电力在核酸-生物大分子复合物中的重要作用，这可能会鼓励新的基因调控、反义治疗和核酸检测策略。
