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  • 1.
    Martín-Yerga, Daniel
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.
    Electrochemical Detection and Characterization of Nanoparticles with Printed Devices2019In: Biosensors, ISSN 2079-6374, Vol. 9, no 2, article id 47Article, review/survey (Refereed)
    Abstract [en]

    Innovative methods to achieve the user-friendly, quick, and highly sensitive detection of nanomaterials are urgently needed. Nanomaterials have increased importance in commercial products, and there are concerns about the potential risk that they entail for the environment. In addition, detection of nanomaterials can be a highly valuable tool in many applications, such as biosensing. Electrochemical methods using disposable, low-cost, printed electrodes provide excellent analytical performance for the detection of a wide set of nanomaterials. In this review, the foundations and latest advances of several electrochemical strategies for the detection of nanoparticles using cost-effective printed devices are introduced. These strategies will equip the experimentalist with an extensive toolbox for the detection of nanoparticles of different chemical nature and possible applications ranging from quality control to environmental analysis and biosensing.

  • 2. Martín-Yerga, Daniel
    et al.
    Costa-García, Agustin
    Unwin, Patrick R
    Correlative Voltammetric Microscopy: Structure-Activity Relationships in the Microscopic Electrochemical Behavior of Screen Printed Carbon Electrodes.2019In: ACS sensors, ISSN 2379-3694Article in journal (Refereed)
    Abstract [en]

    Screen-printed carbon electrodes (SPCEs) are widely used for electrochemical sensors. However, little is known about their electrochemical behavior at the microscopic level. In this work, we use voltammetric scanning electrochemical cell microscopy (SECCM), with dual-channel probes, to determine the microscopic factors governing the electrochemical response of SPCEs. SECCM cyclic voltammetry (CV) measurements are performed directly in hundreds of different locations of SPCEs, with high spatial resolution, using a sub-µm sized probe. Further, the localized electrode activity is spatially-correlated to co-located surface structure information from scanning electron microscopy and micro-Raman spectroscopy. This approach is applied to two model electrochemical processes: hexaammineruthenium (III/II) ([Ru(NH3)6]3+/2+), a well-known outer-sphere redox couple; and dopamine (DA) which undergoes a more complex electron-proton coupled electro-oxidation, with complications from adsorption of both DA and side-products. The electrochemical reduction of [Ru(NH3)6]3+ proceeds fairly uniformly across the surface of SPCEs on the sub-µm scale. In contrast, DA electro-oxidation shows a strong dependence on the microstructure of the SPCE. By studying this process at different concentrations of DA, the relative contributions of (i) intrinsic electrode kinetics and (ii) adsorption of DA are elucidated in detail, as a function of local electrode character and surface structure. These studies provide major new insights on the electrochemical activity of SPCEs and further position voltammetric SECCM as a powerful technique for the electrochemical imaging of complex, heterogeneous and topographically rough electrode surfaces.

  • 3.
    Martín-Yerga, Daniel
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.
    Henriksson, Gunnar
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Cornell, Ann M.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.
    Effects of Incorporated Iron or Cobalt on the Ethanol Oxidation Activity of Nickel (Oxy)Hydroxides in Alkaline Media2019In: Electrocatalysis, ISSN 1868-2529, E-ISSN 1868-5994Article in journal (Refereed)
    Abstract [en]

    Nickel (oxy)hydroxides (NiOxHy) are promising cost-effective materials that exhibit a fair catalytic activity for the ethanol oxidation reaction (EOR) and could be used for sustainable energy conversion. Doping the NiOxHy structure with other metals could lead to enhanced catalytic properties but more research needs to be done to understand the role of the doping metal on the EOR. We prepared NiOxHy films doped with Fe or Co with different metallic ratios by electrodeposition and evaluated the EOR. We found a positive and negative effect on the catalytic activity after the incorporation of Co and Fe, respectively. Our results suggest that Ni atoms are the active sites for the EOR since Tafel slopes were similar on the binary and pristine nickel (oxy)hydroxides and that the formal potential of the Ni(II)/Ni(III) redox couple is a good descriptor for the EOR activity. This work also highlights the importance of controlled metal doping on catalysts and may help in the design and development of improved materials for the EOR.

  • 4.
    Martín-Yerga, Daniel
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry. DropSens, Soc Limitada, Edificio CEEI,Parque Tecnol Asturias, Llanera 33428, Asturias, Spain.
    Perez-Junquera, Alejandro
    DropSens, Soc Limitada, Edificio CEEI,Parque Tecnol Asturias, Llanera 33428, Asturias, Spain..
    Begona Gonzalez-Garcia, Maria
    DropSens, Soc Limitada, Edificio CEEI,Parque Tecnol Asturias, Llanera 33428, Asturias, Spain..
    Hernandez-Santos, David
    DropSens, Soc Limitada, Edificio CEEI,Parque Tecnol Asturias, Llanera 33428, Asturias, Spain..
    Fanjul-Bolado, Pablo
    DropSens, Soc Limitada, Edificio CEEI,Parque Tecnol Asturias, Llanera 33428, Asturias, Spain..
    In Situ Spectroelectrochemical Monitoring of Dye Bleaching after Electrogeneration of Chlorine-Based Species: Application to Chloride Detection2018In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 90, no 12, p. 7442-7449Article in journal (Refereed)
    Abstract [en]

    Spectroelectrochemical techniques are becoming increasingly versatile tools to solve a diverse range of analytical problems. Herein, the use of in situ real-time luminescence spectroelectrochemistry to quantify chloride ions is demonstrated. Utilizing the bleaching effect of chlorine-based electrogenerated products after chloride oxidation, it is shown that the fluorescence of the rhodamine 6G dye decreases proportionally to the initial chloride concentration in solution. A strong decrease of fluorescence is observed in acidic media compared to a lower decrease in alkaline media, which suggests that Cl-2, favorably generated at low pH, could be the main species responsible for the fluorescence loss. This fact is corroborated with chronoamperometric measurements where the complete loss of fluorescence for the bulk solution is achieved. A fast mass transfer is needed to explain this behavior, in agreement with the generation of gaseous species such as Cl-2. Chloride detection was performed in artificial sweat samples in less than 30 s with great accuracy. This electrochemical/optical combined approach allows us to quantify species that are difficult to measure by electrochemistry due to the inadequate resolution of their redox processes or being without significant optical properties.

  • 5.
    Martín-Yerga, Daniel
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry. DropSens S.L., Edificio CEEI, Parque Tecnológico de Asturias, Llanera, Spain.
    Pérez-Junquera, A.
    González-García, M. B.
    Hernández-Santos, D.
    Fanjul-Bolado, P.
    Towards single-molecule: In situ electrochemical SERS detection with disposable substrates2018In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 54, no 45, p. 5748-5751Article in journal (Refereed)
    Abstract [en]

    Dynamic time-resolved Raman spectroelectrochemistry demonstrates the strong influence of nanostructuring and surface charge of in situ activated disposable substrates for SERS detection. Under specific conditions, a large enhancement factor and estimated calculations agree with the feasible detection of only a few molecules, approaching the limit of single-entity detection.

  • 6.
    Pereira da Silva Neves, Marta Maria
    et al.
    Inst Politecn Porto, Inst Super Engn Porto, REQUIMTE LAQV, P-4200072 Porto, Portugal..
    Martín-Yerga, Daniel
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.
    Advanced Nanoscale Approaches to Single-(Bio)entity Sensing and Imaging2018In: Biosensors, ISSN 2079-6374, Vol. 8, no 4, article id 100Article, review/survey (Refereed)
    Abstract [en]

    Individual (bio)chemical entities could show a very heterogeneous behaviour under the same conditions that could be relevant in many biological processes of significance in the life sciences. Conventional detection approaches are only able to detect the average response of an ensemble of entities and assume that all entities are identical. From this perspective, important information about the heterogeneities or rare (stochastic) events happening in individual entities would remain unseen. Some nanoscale tools present interesting physicochemical properties that enable the possibility to detect systems at the single-entity level, acquiring richer information than conventional methods. In this review, we introduce the foundations and the latest advances of several nanoscale approaches to sensing and imaging individual (bio)entities using nanoprobes, nanopores, nanoimpacts, nanoplasmonics and nanomachines. Several (bio)entities such as cells, proteins, nucleic acids, vesicles and viruses are specifically considered. These nanoscale approaches provide a wide and complete toolbox for the study of many biological systems at the single-entity level.

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