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  • Investigation of Doping Effects on the Local Electrochemical Activity of Transition Metal Dichalcogenides 2D Materials

    Walner Costa Silva, Moonjoo Kim, Geovane Arruda de Oliveira, Leandro Vitor da Silva, Emmanuel Batsa Tetteh, Cynthia Marina Rivaldo Gomez, Wellerson dos Reis Ramos, Benjamin Fragneaud, Wolfgang Schuhmann, Carla Santana Santos, Daniel Grasseschi
    Finding strategies to enhance catalysts’ electrochemical activity is based on controlling the material design. Bidimensional materials (2DM) such as MoS2 are explored as catalysts for the hydrogen evolution reaction (HER). A comprehensive study of the effects of doping 2D materials with transition metals based on theoretical predictions in tandem with experimental investigation correlates the doping type to the changes in the electronic and electrochemical activity.
  • Membrane-free Zn hybrid redox flow battery using water-in-salt aqueous biphasic electrolytes

    Sirugaloor Thangavel Senthilkumar, Santiago E. Ibañez, Paula Navalpotro, Eduardo Pedraza, Nagaraj Patil, Jesus Palma, Rebeca Marcilla
    In this study, we develop a membrane-free Zn hybrid redox flow battery (RFB) using an unconventional water-in-salt aqueous biphasic system (WIS-ABS). This membrane-free Zn hybrid battery employs soluble ferrocene (Fc) derivative and Zn salt as the active species in the immiscible catholyte and anolyte, respectively.
  • Au Micro- and Nanoelectrodes as Local Voltammetric pH Sensors During Oxygen Evolution at Electrocatalyst-Modified Electrodes

    Lejing Li, Ndrina Limani, Rajini P Antony, Stefan Dieckhöfer, Carla Santana Santos, Wolfgang Schuhmann
    The scarcity of state-of-the-art oxygen evolution reaction (OER) electrocatalysts has led to intensive research on alternative viable electrocatalytic materials. While activity and cost are the main factors to be sought after, the catalyst stability under harsh acidic conditions is equally crucial.


  • Broadening Applicability of the Poor Academic's Method for Reversing Polarity in Redox Flow Cell Cycling

    Gimena Marin-Tajadura, Eduardo Sánchez-Díez, Virginia Ruiz, Edgar Ventosa
    The use of symmetrical cells is becoming popular for the search of new electroactive materials in redox flow batteries. Unfortunately, low-cost battery cyclers, commonly used for electrochemical battery testing, are not compatible with symmetrical cells since they usually cannot apply negative bias voltages needed for symmetrical cells. The insertion of a Ni−Cd battery in the voltage sensing path is a simple and effective methodology to overcome this limitation for certain battery cyclers.
  • Computer-Aided Design of Membrane-Free Batteries Using Conductor-like Screening Model for Real Solvents

    José Pedro Wojeicchowski, Catarina S. Neves, Paula Navalpotro, Rubén Rubio-Presa, Edgar Ventosa, Rebeca Marcilla, Joao A.P. Coutinho
    Redox Flow Batteries (RFBs), particularly Membrane-Free Flow Batteries based on Aqueous Biphasic Systems (ABSs), are a promising technology for stationary energy storage. However, to prevent the crossover of species, the redox-active compounds used in the catholyte and anolyte must be selectively dissolved, which is currently achieved using expensive physical barriers. In this study, an approach was developed to predict the partition coefficient of redox-active compounds in ABSs formed by ionic liquids or polymers, salt, and water using the Conductor-like Screening Model for Real Solvents (COSMO-RS).
  • Unprecedented Aqueous Solubility of TEMPO and its Application as High Capacity Catholyte for Aqueous Organic Redox Flow Batteries

    Eduardo Pedraza, Carlos de la Cruz, Andreas Mavrandonakis, Edgar Ventosa, Rubén Rubio-Presa, Roberto Sanz, Sirugaloor Thangavel Senthilkumar, Paula Navalpotro, Rebeca Marcilla
    Despite the excellent electrochemical properties of non-functionalized 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), its use in aqueous organic redox flow battery (AORFB) is hindered to date due to its insolubility in water. However, in this study, an unprecedented solubility of 5.6 m is demonstrated in an aqueous solution of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), which is 80 times higher than in water (0.07 m). A computational study reveals that the unique interaction between TEMPO and TFSI is essential to achieve this record solubility.
  • On the Tunability of Toxicity for Viologen-Derivatives as Anolyte for Neutral Aqueous Organic Redox Flow Batteries

    Sandra de la Parra, Juan Antonio Tamayo-Ramos, Rubén Rubio-Presa, Daniel Perez-Antolin, Virginia Ruiz, Prof. Roberto Sanz, Carlos Rumbo, Prof. Edgar Ventosa
    Viologen-derivatives are the most widely used redox organic molecules for neutral pH negative electrolyte of redox flow batteries. However, the long-established toxicity of the herbicide methyl-viologen raises concern for deployment of viologen-derivatives at large scale in flow batteries. Herein, we demonstrate the radically different cytotoxicity and toxicology of a series of viologen-derivatives in in vitro assays using model organisms representative of human and environmental exposure, namely human lung carcinoma epithelial cell line (A549) and the yeast Saccharomyces cerevisiae.
  • Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis

    Carla Santana Santos, Bright Nsolebna Jaato, Ignacio Sanjuán, Wolfgang Schuhmann, and Corina Andronescu
    This review focused in the recent progress in operando scanning electrochemical probe microscopy (SEPM) measurements during electrocatalysis. SEPM techniques can disclose the local electrochemical reactivity of interfaces in single-entity and sub-entity studies. The powerful operando SEPM measurements can correlate electrochemical activity with changes in surface properties as well as provide insight into reaction mechanisms. The capabilities of SEPMs are showcased toward toward the reduction and evolution of O2 and H2 and electrochemical conversion of CO2. Emphasis is given to scanning electrochemical microscopy (SECM), scanning ion conductance microscopy (SICM), electrochemical scanning tunneling microscopy (EC-STM), and scanning electrochemical cell microscopy (SECCM).
  • A neutral pH aqueous biphasic system applied to both static and flow membrane-free battery

    Paula Navalpotro, Santiago E. Ibañez, Eduardo Pedraza, Rebeca Marcilla
    In this contribution to the Energy Storage Materials journal new aqueous biphasic electrolytes with near neutral pH and low cost are prepared. Battery performance shows high efficiency, capacity utilization and stability. Thus, this manuscript represents a breakthrough in the membrane-free battery since it ceases to just be a promising idea demonstrated only in static conditions and becomes a real flow battery.
  • A Systematic Study on the Redox Potentials of Phenazine-derivatives in Aqueous Media: A Combined Computational and Experimental Work

    Carlos de la Cruz, Roberto Sanz, Anisley Suárez, Edgar Ventosa, Rebeca Marcilla, Andreas Mavrandonakis
    Phenazines are an emerging class of organic compounds that have been recently utilized in aqueous redox flow batteries, a promising technology for large-scale energy storage. A virtual screening based on density functional theory calculations is used to investigate the redox potentials of around 100 phenazine derivatives in aqueous media containing various electron-donating or electron-withdrawing groups at different positions.
  • Addressing Practical Use of Viologen-Derivatives in Redox Flow Batteries through Molecular Engineering

    Ruben Rubio-Presa, Lara Lubian, Mario Borlaf, Edgar Ventosa, Roberto Sanz
    In practical scenarios, viologen-derivatives face an accelerated degradation in the unavoidable presence of traces of oxygen in large-scale redox flow batteries. Herein, we confirm the primary degradation mechanism and propose a straightforward, cheap, and fast method to evaluate the stability of viologen-derivatives toward this degradation. A new viologen-derivative is designed and synthesized to illustrate how molecular engineering can be used to improve stability.