3D electrogenerated chemiluminescence: from surface-confined reactions to bulk emission

Among luminescence techniques, electrogenerated chemiluminescence (ECL) provides a unique level of manipulation of the luminescent process by controlling the electrochemical trigger. Despite its attractiveness, ECL is by essence a 2D process where light emission is strictly confined to the electrode surface. To overcome this intrinsic limitation, we added a new spatial dimension to the ECL process by generating 3D ECL at the level of millions of micro-emitters dispersed in solution. Each single object is addressed remotely by bipolar electrochemistry and they generate collectively the luminescence in the bulk. Therefore, the entire volume of the solution produces light. To illustrate the generality of this concept, we extended it to a suspension of multi-walled carbon nanotubes where each one acts as an individual ECL nano-emitter. This approach enables a change of paradigm by switching from a surface-limited process to 3D electrogenerated light emission

Infrared photoinduced electrochemiluminescence microscopy of single cells

Electrochemiluminescence (ECL) is evolving rapidly from a purely analytical technique into a powerful microscopy. Herein, we report the imaging of single cells by photoinduced ECL (PECL; λem = 620 nm) stimulated by an incident near-infrared light (λexc = 1050 nm). The cells were grown on a metal–insulator–semiconductor (MIS) n-Si/SiOx/Ir photoanode that exhibited stable and bright PECL emission. The large anti-Stokes shift allowed for the recording of well-resolved images of cells with high sensitivity. PECL microscopy is demonstrated at a remarkably low onset potential of 0.8 V; this contrasts with classic ECL, which is blind at this potential. Two imaging modes are reported: (i) photoinduced positive ECL (PECL+), showing the cell membranes labeled with the [Ru(bpy)3]2+ complex; and (ii) photoinduced shadow label-free ECL (PECL−) of cell morphology, with the luminophore in the solution. Finally, by adding a new dimension with the near-infrared light stimulus, PECL microscopy should find promising applications to image and study single photoactive nanoparticles and biological entities

Supplementary data for the article: Habtamu, H. B.; Sentic, M.; Silvestrini, M.; De Leo, L.; Not, T.; Arbault, S.; Manojlovic, D.; Sojic, N.; Ugo, P. A Sensitive Electrochemiluminescence Immunosensor for Celiac Disease Diagnosis Based on Nanoelectrode Ensembles. Analytical Chemistry 2015, 87 (24), 12080–12087. https://doi.org/10.1021/acs.analchem.5b02801

Supporting information for: [https://doi.org/10.1021/acs.analchem.5b02801]Related to published version: [http://cherry.chem.bg.ac.rs/handle/123456789/2014

Luminescent Metal-Organic Frameworks for Electrochemiluminescent Detection of Water Pollutants

Modern lifestyle has increased our utilization of pollutants such as heavy metals, aromatic 17 compounds, and contaminants of rising concern involving pharmaceutical and personal products 18 and other materials that may have an important environmental impact. Especially, the ultimate re-19 sults of intense use of highly stable materials, such as heavy metals and chemical restudies are that 20 they turn into waste materials which, when discharged, accumulate in the environment water bod-21 ies. In this context, the present review presents application of metal-organic frameworks (MOFs) in 22 electrochemiluminescent (ECL) sensing for water pollutant detection. MOF composites applied as 23 innovative luminophore or luminophore carriers, materials for electrode modification and enhance-24 ment of co-reaction in ECL sensors have enabled sensitive monitoring of some most common con-25 taminants of emerging concern such as heavy metals, volatile organic compounds, pharmaceuticals, 26 industrial chemicals and cyanotoxins. Moreover, we provide future trends and prospects associated 27 with ECL MOF-composites for environmental sensing

Supplementary data for the article: Habtamu, H. B.; Sentic, M.; Silvestrini, M.; De Leo, L.; Not, T.; Arbault, S.; Manojlovic, D.; Sojic, N.; Ugo, P. A Sensitive Electrochemiluminescence Immunosensor for Celiac Disease Diagnosis Based on Nanoelectrode Ensembles. Analytical Chemistry 2015, 87 (24), 12080–12087. https://doi.org/10.1021/acs.analchem.5b02801

Supporting information for: [https://doi.org/10.1021/acs.analchem.5b02801]Related to published version: [http://cherry.chem.bg.ac.rs/handle/123456789/2014

Supplementary data for article: Filipović, N. R.; Elshaflu, H.; Grubišić, S.; Jovanović, L. S.; Rodić, M.; Novaković, I.; Malešević, A.; Djordjević, I. S.; Li, H.; Šojić, N.; et al. Co(III) Complexes of (1,3-Selenazol-2-Yl)Hydrazones and Their Sulphur Analogues. Dalton Transactions 2017, 46 (9), 2910–2924. https://doi.org/10.1039/c6dt04785h

Supplementary material for: [https://doi.org/10.1039/c6dt04785h]Related to published version: [http://cherry.chem.bg.ac.rs/handle/123456789/2430

Supplementary data for article: Filipović, N. R.; Elshaflu, H.; Grubišić, S.; Jovanović, L. S.; Rodić, M.; Novaković, I.; Malešević, A.; Djordjević, I. S.; Li, H.; Šojić, N.; et al. Co(III) Complexes of (1,3-Selenazol-2-Yl)Hydrazones and Their Sulphur Analogues. Dalton Transactions 2017, 46 (9), 2910–2924. https://doi.org/10.1039/c6dt04785h

Supplementary material for: [https://doi.org/10.1039/c6dt04785h]Related to published version: [http://cherry.chem.bg.ac.rs/handle/123456789/2430

Advances in bipolar electrochemiluminescence for the detection of biorelevant molecular targets

Bipolar electrochemistry (BPE) contrasts very much with conventional electrochemistry because it is based on the control of the solution potential instead of the working electrode potential. In a typical setup, a piece of conducting materials is immersed in an electrolyte and submitted to an electric field. Such conditions split the interfacial nature of the materials into cathodic and anodic domains where electrochemical reactions can readily take place. BPE has many potential applications, and the present contribution aims to focus on recent analytical applications that involve electrogenerated chemiluminescence (ECL) detection. ECL is a special case of luminescence where the excited state of the luminophore is populated after a sequence of reaction that is triggered by an initial electron transfer step occurring at the electrode surface. The coupling between BPE and ECL is a powerful approach because it provides a unique opportunity to combine the intrinsic advantages of both techniques. BPE enables the spatial separation of sensing and reporting poles, whereas ECL provides a simple and sensitive visual readout. This opinion article will describe the experimental possibilities and the most recent applications of BPE/ECL coupling for the detection of biorelevant molecular targets.Peer-reviewed version: [http://cherry.chem.bg.ac.rs/handle/123456789/3046

Glucose sensing by electrogenerated chemiluminescence of glucose-dehydrogenase produced NADH on electrodeposited redox hydrogel

In this work, we report a new sensing approach based on electrogenerated chemiluminescence (ECL) in an electrodeposited redox hydrogel using glucose dehydrogenase as a model system. The ECL-hydrogel films were electrodeposited by potential cycling of a PBS solution containing [poly(4-vinylpyridine)Ru(2,2'-bipyridine)(2) Cl-](+/2+). The film was easily prepared in a rapid, reproducible and well-controlled one-step procedure. The deposited hydrogel film is permeable to water-soluble chemicals and biochemicals, like enzyme substrates and coenzymes. Electrochemistry and ECL of NADH were studied at the level of the hydrogel film. Results indicate that ECL emission occurs at a relatively low anodic potential compared to the classical Ru(bipy)(3)(2+) complex. This is an important advantage since the measurements performed with the ECL hydrogel are thus less sensitive to interfering species. An ECL oxidative-reductive mechanism is presented for the ECL-hydrogel. Then we showed that the intensity of the ECL of NADH produced by the enzymatic activity varies with the enzyme substrate concentration. Such sensing approach combines enzymatic selectivity with the ECL advantages at low oxidation potential. (C) 2011 Elsevier B.V. All rights reserved