Light conversion by photoinduced-electrochemiluminescence – LiCORN
LiCORN
Light COnveRsioN by photoinduced-electrochemiluminescence
LiCORN aims to combine two opposite concepts: ECL & semi-conductor photoelectrochemistry to create a new field of research referred to as photoinduced-ECL.
Electrochemiluminescence (ECL) is the emission of light caused by the excited state of a luminophore that is generated by an electrochemical reaction at an electrode surface. This physicochemical phenomenon has become a powerful tool for analytical chemistry as it provides outstanding benefits over photoluminescence and chemiluminescence due to its versatility, its simple optical setup, good spatial and temporal control as well its excellent sensitivity (absence of background signal). ECL is commonly used for many clinical lab applications, including DNA analysis and a wide range of immunoassays currently commercialized for cardiac and infectious<br />diseases, thyroid, Alzheimer's disease, tumor markers, etc. ECL involves highly exergonic redox reactions and is a manifestation of the inverted Marcus region. Therefore, it implies usually electrochemical reactions occurring at very negative or very positive potentials. It is interesting to note that, fundamentally, in ECL, the electrode/electrolyte interface can be considered as a light emitter. This is opposed to what happens in another type of photoelectrochemistry, called “semiconductor (SC) photoelectrochemistry”, in which the electrode surface is a light absorber. The main principle of SC photoelectrochemistry consists in employing photogenerated minority carriers within a depleted SC for a redox reaction at the solid/liquid interface (holes (h+) for an n-type photoanode and electrons (e-) for a p-type photocathode). This concept has proved to be very useful because it allows triggering electrochemical reactions with a lower potential. In particular, driven by the environmental crisis, SC photoelectrochemistry has lately attracted a lot of attention in the context of solar conversion research with applications in sunlight assisted photoelectrochemical water splitting, CO2 reduction, and N2 fixation. LiCORN aims to combine ECL with SC photoelectrochemistry in order to create a new field of research that we refer to as “photoinduced-electrochemiluminescence” (P-ECL). Note that P-ECL fundamentally differs from the field of photoinduced chemiluminescence (CL), in which CL is triggered by illumination of dissolved chemicals.<br />The objective of LiCORN is to provide crucial fundamental insights on P-ECL and to evaluate its potential for<br />imaging. To do this, the LiCORN project has three main objectives, namely: (i) the in-depth elucidation of a highly robust model system to acquire a considerable amount of knowledge on P-ECL (WP1); (ii) the development of key demonstrators to explore the versatility of this concept (WP2 and WP3); and (iii) the use of P-ECL in a proof-of-concept device for assessing its application potential (WP4).
LiCORN est divisé en cinq workpackages (WP, présentés dans le schéma 1), qui sont eux-mêmes subdivisés en un total de 8 tâches, qui impliquent toutes plusieurs partenaires de l'équipe LiCORN (ISCR, Rennes / ISM, Bordeaux, FOTON, Rennes, et CiNAM, Marseille). Le premier WP, WP0, concerne la coordination du projet qui sera assurée par le partenaire1. Les quatre autres WP (WP1 - WP4) constituent le noyau scientifique de LiCORN, et chaque partenaire est responsable d'un WP scientifique. Les WP1, WP3 et la majeure partie du WP2 peuvent être réalisés indépendamment. Le WP4 est le seul WP qui dépend d'autres tâches et sera exécuté au dernier stade du projet.
The LiCORN project has already resulted in several important achievements, among which :
-A considerable increase in the performance of the photoelectrodes used for the conversion of infrared photons into visible light by P-ECL ( i.e., the phenomenon at the heart of the LiCORN project). Indeed, before LiCORN, the P-ECL had been reported for 15 min. By using appropriate materials, the consortium has shown that this conversion can be performed for more than 35 h (Angew. Chem. Int. Ed. 2022, 61, e202201865). We believe that this breakthrough will allow us to unlock the technological locks for the continuation of the LiCORN project.
-Several fundamental aspects have been studied such as: -the use of ECL to activate semiconductors (Cell Rep. Phys. Sci. 2021, 2, 100670), -the development of a luminescence amplification system (Electrochim. Acta 2021, 381, 138238), -a new cathode system (Chem. Commun., 2022, 58, 6686) and -wireless P-ECL addressable systems (J. Phys. Chem. Lett. 2022, 13, 5538).
-A compilation of the state of the art has been made on electrochemiluminescence with semiconductor materials (Chem. Sci. 2022, 13, 2528)
We plan to develop an IR imaging system and applications in microscopy.
1. Yu, H. Saada, N. Sojic, G. Loget, Photoinduced electrochemiluminescence at nanostructured hematite electrodes, Electrochim. Acta 2021, 381, 138238
hal-03190652
doi.org/10.1016/j.electacta.2021.138238
2. Y. Zhao, J. Yu, J.-F. Bergamini, Y. Léger, N. Sojic, G. Loget, Photoelectrochemistry at semiconductor/liquid interfaces triggered by electrochemiluminescence, Cell Rep. Phys. Sci. 2021, 2, 100670
hal-03468707
doi.org/10.1016/j.xcrp.2021.100670
3. Y. Zhao, L. Bouffier, G. Xu, G. Loget, N. Sojic, Electrochemiluminescence at semiconductor (nano)materials, Chem. Sci. 2022, 13, 2528–2550
COVER
hal-03592698
doi.org/10.1039/d1sc06987j
4. Y. Zhao, J. Descamps, S. Ababou-Girard, J.-F. Bergamini, L. Santinacci, Y. Léger, N. Sojic, G. Loget, Metal-insulator-semiconductor anodes for ultrastable and site-selective upconversion photoinduced electrochemiluminescence,
Angew. Chem. Int. Ed. 2022, 61, 20, e202201865
VIP ARTICLE
hal-03629802
doi.org/10.1002/anie.202201865
5. J. Descamps, Y. Zhao, J. Yu, G. Xu, Y. Léger, G. Loget, N. Sojic, Anti-Stokes photoinduced electrochemiluminescence at a photocathode, Chem. Commun. 2022, 58, 6686-6688
COVER
hal-03688103
doi.org/10.1039/d2cc01804g
6. Y. Zhao, J. Descamps, B. Le Corre, Y. Léger, A. Kuhn, N. Sojic, G. Loget, Wireless Anti-Stokes Photo-induced Electrochemiluminescence, J. Phys. Chem. Lett. in press, 2022, 13, 5538–5544
doi.org/10.1021/acs.jpclett.2c01512
Electrochemiluminescence (ECL) consists of the emission of light induced by the excited state of a luminophore, generated at an electrode surface. On the other hand, photoelectrochemistry at illuminated semiconductor (SC) relies on employing photogenerated minority carriers within a depleted SC in order to decrease the potential required to trigger an electrochemical reaction. The LiCORN project aims to combine ECL with SC photoelectrochemistry -two fields that are currently of considerable scientific interest- to create a new field of research referred to as “photoinduced-electrochemiluminescence” (P-ECL), whose basic principle has been recently demonstrated by two partners of LiCORN. The objective of this project is to provide crucial fundamental insights on P-ECL and to evaluate its potential for detection and imaging. To do so, the LiCORN team consists of four expert partners, combining the complementary skills in SC photoelectrochemistry, ECL, optics and materials science.
Project coordination
INSTITUT DES SCIENCES CHIMIQUES DE RENNES (Organisme de recherche)
The author of this summary is the project coordinator, who is responsible for the content of this summary. The ANR declines any responsibility as for its contents.
Partnership
Inst.FOTON Institut Fonctions Optiques pour les Technologies de l'informatiON
ISCR INSTITUT DES SCIENCES CHIMIQUES DE RENNES
ISM INSTITUT DES SCIENCES MOLECULAIRES
CINaM Centre National de la Recherche Scientifique Délégation Provence et Corse _ Centre Interdisciplinaire de Nanoscience de Marseille
Help of the ANR 509,760 euros
Beginning and duration of the scientific project:
- 42 Months