Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 14, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202200187
Keywords
Electrochemiluminescence; Kinetics; Single Molecules; Super-Resolution Imaging
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Funding
- Natural Science Foundation of Zhejiang Province [LR20B050002]
- National Natural Science Foundation of China [21974123]
- National Key R&D Program of China [2020YFA0211200]
- Hundreds Program of Zhejiang University
- ITO
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Here, we demonstrate super-resolution imaging of Ru(bpy)(3)(2+) reactions on Au plates using single-molecule electrochemiluminescence microscopy, achieving high spatial resolution and sensitivity to single photons. The spatiotemporally resolved dynamic structure-activity relationship on Au plates reveals the importance of catalyst restructuring in determining reactivity.
Classical electrochemical characterization tools cannot avoid averaging between the active reaction sites and their support, thus obscuring their intrinsic roles. Single-molecule electrochemical techniques are thus in high demand. Here, we demonstrate super-resolution imaging of Ru(bpy)(3)(2+) based reactions on Au plates using single-molecule electrochemiluminescence microscopy. By converting electrochemical signals into optical signals, we manage to achieve the ultimate sensitivity of single-entity chemistry, that is directly resolving the single photons from individual electrochemical reactions. High spatial resolution, up to 37 nm, further enables mapping Au chemical activity and the reaction kinetics. The spatiotemporally resolved dynamic structure-activity relationship on Au plates shows that the restructuring of catalysts plays an important role in determining the reactivity. Our approach may lead to gaining new insights towards evaluating and designing electrocatalytic systems.
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