Photoinduced Electrochemiluminescence at Silicon Electrodes in Water

Abstract

We introduce the photoinduced electrochemiluminescence (P-ECL) of the model ECL system involving the simultaneous oxidation of [Ru­(bpy)3]2+ and tri-n-propylamine (TPrA). This system classically requires highly anodic potentials of greater than +1 V vs SCE for ECL generation. In the reported approach, the ECL emission is triggered by holes (h+) photogenerated in an n-type semiconductor (SC) electrode, which is normally highly challenging because of competing photocorrosion occurring on SC electrodes in aqueous electrolytes. We employ here Si-based tunnel electrodes protected by few-nanometer-thick SiO x and Ni stabilizing thin films and demonstrate that this construct allows generation of P-ECL in water. This system is based on an upconversion process where light absorption at 810 nm induces ECL emission (635 nm) at a record low electrochemical potential of 0.5 V vs SCE. Neither this excitation wavelength nor this low applied potential is able to stimulate ECL light if applied alone, but their synergetic action leads to stable and intense ECL emission in water. This P-ECL strategy can be extended to other luminophores and is promising for ultrasensitive detection and light-addressable and imaging devices.

Advances in chemiluminescence and electrogenerated chemiluminescence based on silicon nanomaterials

“…Increasingly, ECL sensors based on silicon nanomaterials that show high sensitivity and selectivity have been designed. More recently, silicon‐based materials (close‐packed monolayered SiO 2 ‐ nanomembrane [ 96 ] and n‐Si/SiOx/Ni [ 97 ] ) have been fabricated as novel ECL electrodes in subtle ways. About a 77‐fold ECL enhancement in the classic Ru(bpy) 3 2+ –TPrA system was obtained on SiO 2 ‐nanomembrane electrodes.…”

Electrochemiluminescence Waveguide in Single Crystalline Molecular Wires

“…This feature indeed has stimulated research focus on ECL‐based microscopy for imaging of sensing‐array, latent fingermarks, single micro‐/nanoentities, proteins on the cell membrane and subcellular structures . In addition, a lot of novel ECL‐related concepts and techniques have also been developed more recently, such as self‐enhanced ECL, potential‐resolved multicolor ECL, aggregation‐induced ECL (AIECL), surface plasmon resonance modulated ECL, photoinduced ECL and circularly‐polarized ECL . In this work we report the first observation of ECL waveguide (ECLW) in single crystalline molecular wires of tris(1‐phenylisoqsuinoline‐ C 2 , N )iridium (III) (Ir(piq) 3 ).…”

Fluorescent Noble Metal Nanoclusters Loaded Protein Hydrogel Exhibiting Anti‐Biofouling and Self‐Healing Properties for Electrochemiluminescence Biosensing Applications

“…[ 1–3 ] By far, remarkable efforts have been made to develop various types of ECL based biosensing systems, [ 4,5 ] and the recent introduction of new ECL materials or mechanisms, such as metal‐organic frameworks, aggregation‐induced emission luminogens or single atom catalysts, further improved the performance and application ranges of ECL based biosensing systems. [ 6–11 ] However, as a method extremely sensitive to the state of the electrode surface, nonspecific adsorption of biological macromolecules, in particular proteins, and physical scratches of the electrode surfaces, during the sensing of complex biological samples, severely affects the accuracy and practical applicability of the ECL biosensing systems. [ 12 ] In order to meet the requirements of anti‐interference and long‐term application in practical biosensing applications, it is highly demanded to develop ECL biosensing systems with anti‐biofouling and self‐healing properties.…”