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作 者:Rong Jin Yu Li Yanyan Xu Lei Cheng Dechen Jiang
机构地区:[1]State Key Laboratory of Analytical Chemistry for Life Science and School of Chemistry and Chemical Engineering,Nanjing University,Nanjing,China [2]College of Engineering and Technology,Southwest University,Chongqing,China
出 处:《Research》2025年第1期975-983,共9页研究(英文)
基 金:supported by the National Natural Science Foundation of China(nos.22025403,22304079,and 22327802);Jiangsu Social Development Project(BE2022794);Jiangsu Funding Program for Excellent Postdoctoral Talent(2023ZB543).
摘 要:Stereoscopic imaging of single molecules at the plasma membrane of single cell requires spatial resolutions in 3 dimensions(x-y-z)at 10-nm level,which is rarely achieved using most optical super-resolution microscopies.Here,electrochemical stereoscopic microscopy with a detection limit down to a single molecule is achieved using a photoreduction-assisted cycle inside a 20-nm gel electrolyte nanoball at the tip of a nanopipette.On the basis of the electrochemical oxidation of Ru(bpy)_(3)^(2+)into Ru(bpy)33+followed by the reduction of Ru(bpy)_(3)^(3+)into Ru(bpy)_(3)^(2+)by photogenerated isopropanol radicals,a charge of 1.5 fC is obtained from the cycling electron transfers involving one Ru(bpy)_(3)^(2+/3+)molecule.By using the nanopipette to scan the cellular membrane modified with Ru(bpy)_(3)^(2+)-tagged antibody,the morphology of the cell membrane and the distribution of carcinoembryonic antigen(CEA)on the membrane are electrochemically visualized with a spatial resolution of 14 nm.The resultant stereoscopic image reveals more CEA on membrane protrusions,providing direct evidence to support easy access of membrane CEA to intravenous antibodies.The breakthrough in single-molecule electrochemistry at the cellular level leads to the establishment of high-resolution 3-dimensional single-cell electrochemical microscopy,offering an alternative strategy to remedy the imperfection of stereoscopic visualization in optical microscopes.
关 键 词:stereoscopic imaging electrochemical oxidation plasma membrane photoreduction assisted electrochemistry single molecules stereoscopic microscopy
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