Hydrogen evolution at polarised liquid/liquid interfaces catalyzed by molybdenum disulfide

Hatay, İmren; Ge, Pei Yu; Vrubel, Heron; Hu, Xile; Girault, Hubert H.

doi:10.1039/c1ee01996a

Cited by 77 publications

(101 citation statements)

References 25 publications

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“…AuNPs were charged by an electron donor (DMFc) in the organic phase that acts as a barrier-free shortcut for electrons to the aqueous phase. or anaerobic conditions, was immediately imposed by the DMFc +/0 redox couple on contact due to an electrostatic charging process (Scheme 2): reduction reaction, DMFc + was quantified from the magnitude of its absorption peak using the Beer-Lambert Law; l max for DMFc + is 779 nm and the extinction coefficient of DMFc + in a similar organic phase, 1,2-dichloroethane, is 0.632 mM À1 cm À1 [21]. Inset: Characteristic UV/vis spectra of the two distinguishing absorption peaks of the I 3 -cation in the aqueous phase diluted by half (l max = 288 and 354 nm) formed after interaction of the H 2 O 2 generated during the biphasic O 2 reduction reaction with an excess of KI over 30 minutes [18].…”

Section: Mechanism Of Biphasic O 2 Reduction By Interfacial Redox Catmentioning

confidence: 99%

“…A burgeoning area of research is concerned with the biphasic electrocatalysis of redox reactions of interest for energy research, including the oxygen (O 2 ) reduction reaction (ORR) [9][10][11][12][13][14][15][16][17][18][19] and the hydrogen (H 2 ) evolution reaction (HER) [20][21][22][23][24][25][26][27][28], using soft interfaces functionalized with molecular species, metallic NPs or inorganic non-precious metal-based materials. The use of adsorbed solid particulate electrocatalysts at electrochemically polarisable soft interfaces has recently been reviewed by Dryfe and co-workers [29].…”

Section: Introductionmentioning

confidence: 99%

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Gold Nanofilm Redox Catalysis for Oxygen Reduction at Soft Interfaces

Smirnov

Peljo

Scanlon

et al. 2016

Electrochimica Acta

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A B S T R A C TFunctionalization of a soft or liquid-liquid interface by a one gold nanoparticle thick "nanofilm" provides a conductive pathway to facilitate interfacial electron transfer from a lipophilic electron donor to a hydrophilic electron acceptor in a process known as interfacial redox catalysis. The gold nanoparticles in the nanofilm are charged by Fermi level equilibration with the lipophilic electron donor and act as an interfacial reservoir of electrons. Additional thermodynamic driving force can be provided by electrochemically polarising the interface. Using these principles, the biphasic reduction of oxygen by a lipophilic electron donor, decamethylferrocene, dissolved in a,a,a-trifluorotoluene was catalysed at a gold nanoparticle nanofilm modified water-oil interface. A recently developed microinjection technique was utilised to modify the interface reproducibly with the mirror-like gold nanoparticle nanofilm, while the oxidised electron donor species and the reduction product, hydrogen peroxide, were detected by ion transfer voltammetry and UV/vis spectroscopy, respectively. Metallization of the soft interface allowed the biphasic oxygen reduction reaction to proceed via an alternative mechanism with enhanced kinetics and at a significantly lower overpotential in comparison to a bare soft interface. Weaker lipophilic reductants, such as ferrocene, were capable of charging the interfacial gold nanoparticle nanofilm but did not have sufficient thermodynamic driving force to significantly elicit biphasic oxygen reduction.

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Section: Mechanism Of Biphasic O 2 Reduction By Interfacial Redox Catmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Gold Nanofilm Redox Catalysis for Oxygen Reduction at Soft Interfaces

Smirnov

Peljo

Scanlon

et al. 2016

Electrochimica Acta

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“…Recently, it has been shown that hydrogen evolution reaction (HER) occurs at the 1,2-dichloroethane (DCE)| water interface under anaerobic conditions, with decamethylferrocene (DMFc) as a reducing agent present in the organic phase [3][4][5]. This reaction is significantly accelerated by the presence of micro-or nanoparticles [6,7].…”

Section: Introductionmentioning

confidence: 99%

Scanning electrochemical microscopy determination of hydrogen flux at liquid|liquid interface with potentiometric probe

Jedraszko¹,

Nogala²,

Adamiak³

et al. 2014

Electrochemistry Communications

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Scanning electrochemical microscopy potentiometric determination of local hydrogen concentration and its flux next to the liquid|liquid interface was demonstrated. This method is based on the shift of open circuit potential of Pt-based reversible hydrogen electrode. The detection system was verified with a system generating hydrogen under galvanostatic conditions. Then, it was applied to aqueous|1,2-dichloroethane interface where hydrogen is produced with decamethylferrocene as electron donor.

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“…have been used in the redox electrocatalysis of, for example, oxygen reduction, 18,26 hydrogen evolution 25,27,28 and metal deposition at the ITIES.…”

Section: Introductionmentioning

confidence: 99%

Electrovariable gold nanoparticle films at liquid–liquid interfaces: from redox electrocatalysis to Marangoni-shutters

et al. 2017

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Control over the physical properties of nanoparticle assemblies at a liquid-liquid interface is a key technological advancement to realize the dream of smart electrovariable nanosystems.Electrified interfaces, such as the interface between two immiscible electrolytes solutions (ITIES), are almost an ideal platform for realizing this dream. Here, we show that the Galvani potential difference across soft interfaces can be effectively used to manipulate: (i) the reactivity of gold nanoparticle assemblies through varying the Fermi level (both chemically and electrochemically); (ii) the location distribution of the nanoparticles at the liquid-liquid interface. In the first case, in addition to our previous studies on electron transfer reactions (ET) across the ITIES, we used intensity modulated photocurrent spectroscopy (IMPS) to study the kinetics of photo-induced electrochemical reactions at the ITIES. As expected, the direct adsorption of gold nanoparticles at the interface modifies the kinetics of the ET reaction (socalled, interfacial redox electrocatalysis), however it did not lead to an increased photocurrent by "plasmonic enhancement". Rather, we found that the product separation depends on double layer effects while the product recombination is controlled by the Galvani potential difference between the two phases. In the second case, we demonstrated that polarizing the ITIES caused migration of gold nanoparticles from the middle region of the cell to its periphery. We called such systems "Marangoni-type shutters". This type of electrovariable plasmonic system did not experience diffusion limitation in terms of the adsorption/ desorption of nanoparticles and the entire movement of nanoparticle assemblies happened almost instantly (within a second). It opens a fresh view on electrovariable plasmonics and presents new opportunities to create smart nanosystems at the ITIES driven with an electric field.

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Hydrogen evolution at polarised liquid/liquid interfaces catalyzed by molybdenum disulfide

Cited by 77 publications

References 25 publications

Gold Nanofilm Redox Catalysis for Oxygen Reduction at Soft Interfaces

Gold Nanofilm Redox Catalysis for Oxygen Reduction at Soft Interfaces

Scanning electrochemical microscopy determination of hydrogen flux at liquid|liquid interface with potentiometric probe

Electrovariable gold nanoparticle films at liquid–liquid interfaces: from redox electrocatalysis to Marangoni-shutters

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