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      Self‐assembly Induced Enhanced Electrochemiluminescence of Copper Nanoclusters Using DNA Nanoribbon Templates

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          Abstract

          Copper nanoclusters (CuNCs) are attractive electrochemiluminescence (ECL) emitters as Cu is comparatively inexpensive, nontoxic, and highly abundant. However, their ECL yield is relatively low. Herein, we report that orderly self‐assembly of CuNCs using DNA nanoribbon as the template (DNR/CuNCs) conferred the CuNCs with improved ECL properties compared with individual CuNCs in both annihilation and co‐reactant processes. The DNR/CuNCs resulted in a high ECL yield of 46.8 % in K 2S 2O 8, which was ≈68 times higher than that of individual CuNCs. This strategy was successfully extended to other ECL emitters, such as gold nanoclusters and the Ru(bpy) 3 2+/TPrA system. Furthermore, as an application of DNR/CuNCs, a DNR/CuNC‐based ECL biosensor with higher sensitivity was constructed for dopamine determination (two orders of magnitude lower than that previously reported), showing that DNR/CuNCs have a potential for application in ECL bioanalysis as a new type of superior luminophore candidate.

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          Most cited references96

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          Folding DNA to create nanoscale shapes and patterns.

          'Bottom-up fabrication', which exploits the intrinsic properties of atoms and molecules to direct their self-organization, is widely used to make relatively simple nanostructures. A key goal for this approach is to create nanostructures of high complexity, matching that routinely achieved by 'top-down' methods. The self-assembly of DNA molecules provides an attractive route towards this goal. Here I describe a simple method for folding long, single-stranded DNA molecules into arbitrary two-dimensional shapes. The design for a desired shape is made by raster-filling the shape with a 7-kilobase single-stranded scaffold and by choosing over 200 short oligonucleotide 'staple strands' to hold the scaffold in place. Once synthesized and mixed, the staple and scaffold strands self-assemble in a single step. The resulting DNA structures are roughly 100 nm in diameter and approximate desired shapes such as squares, disks and five-pointed stars with a spatial resolution of 6 nm. Because each oligonucleotide can serve as a 6-nm pixel, the structures can be programmed to bear complex patterns such as words and images on their surfaces. Finally, individual DNA structures can be programmed to form larger assemblies, including extended periodic lattices and a hexamer of triangles (which constitutes a 30-megadalton molecular complex).
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            DNA nanotechnology

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              Electrochemiluminescence (ECL).

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                Author and article information

                Contributors
                Journal
                Angewandte Chemie International Edition
                Angew Chem Int Ed
                Wiley
                1433-7851
                1521-3773
                May 15 2023
                April 17 2023
                May 15 2023
                : 62
                : 21
                Affiliations
                [1 ] Xi'an Key Laboratory of Functional Supramolecular Structure and Materials Key Laboratory of Synthetic and Natural Functional Molecule of Ministry of Education College of Chemistry & Materials Science Northwest University Xi'an Shaanxi 710127 China
                [2 ] The Interdisciplinary Research Center Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 China
                [3 ] Institute of Materials Biology Department of Chemistry College of Science Shanghai University Shanghai 200444 China
                [4 ] Zhangjiang Laboratory Shanghai 201210 China
                [5 ] School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine Shanghai Jiao Tong University Shanghai 200240 China
                Article
                10.1002/anie.202300893
                b75543be-4b5f-4f22-9879-35d84fa852f5
                © 2023

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