Electrochemical hydrogen production on a metal-free polymer

Valiollahi, Roudabeh; Vagin, Mikhail; Gueskine, Viktor; Singh, Amritpal; Grigoriev, S.A.; Pushkarev, Artem S.; Pushkareva, I. V.; Fahlman, Mats; Liu, Xianjie; Khan, Ziyauddin; Berggren, Magnus; Zozoulenko, Igor; Crispin, Xavier

doi:10.1039/c9se00687g

Cited by 26 publications

(28 citation statements)

References 68 publications

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“…The two‐electron hydrogen‐evolution reaction (Equation ( 4 )) can happen on PEDOT, however only at very low pH values. [ 40 ] This reaction is not efficient at pH values exceeding 3. Therefore, under neutral pH conditions, Equation ( 1 ) can be expected to predominate on PEDOT.…”

Section: Resultsmentioning

confidence: 99%

Faradaic Pixels for Precise Hydrogen Peroxide Delivery to Control M‐Type Voltage‐Gated Potassium Channels

et al. 2021

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H2O2 plays a significant role in a range of physiological processes where it performs vital tasks in redox signaling. The sensitivity of many biological pathways to H2O2 opens up a unique direction in the development of bioelectronics devices to control levels of reactive‐oxygen species (ROS). Here a microfabricated ROS modulation device that relies on controlled faradaic reactions is presented. A concentric pixel arrangement of a peroxide‐evolving cathode surrounded by an anode ring which decomposes the peroxide, resulting in localized peroxide delivery is reported. The conducting polymer (poly(3,4‐ethylenedioxythiophene) (PEDOT), is exploited as the cathode. PEDOT selectively catalyzes the oxygen reduction reaction resulting in the production of hydrogen peroxide (H2O2). Using electrochemical and optical assays, combined with modeling, the performance of the devices is benchmarked. The concentric pixels generate tunable gradients of peroxide and oxygen concentrations. The faradaic devices are prototyped by modulating human H2O2‐sensitive Kv7.2/7.3 (M‐type) channels expressed in a single‐cell model (Xenopus laevis oocytes). The Kv7 ion channel family is responsible for regulating neuronal excitability in the heart, brain, and smooth muscles, making it an ideal platform for faradaic ROS stimulation. The results demonstrate the potential of PEDOT to act as an H2O2 delivery system, paving the way to ROS‐based organic bioelectronics.

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Section: Resultsmentioning

confidence: 99%

Faradaic Pixels for Precise Hydrogen Peroxide Delivery to Control M‐Type Voltage‐Gated Potassium Channels

et al. 2021

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“…Both are sluggish at inert electrodes and thus require electrocatalytic, traditionally noble metal, electrodes. Experimentally, both HER and ORR at rigorously metal-free PEDOT were performed in many groups around the world. − However, the mechanisms of these reactions at PEDOT are not necessarily transposed from those established for other electrode materials. Quantum-chemical modeling is an indispensable tool in uncovering these mechanisms. ,, …”

Section: Electrochemistry and Catalytic Action: Oxygen Reduction Reac...mentioning

confidence: 99%

Electronic, Optical, Morphological, Transport, and Electrochemical Properties of PEDOT: A Theoretical Perspective

et al. 2021

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Among all conducting polymers, PEDOT or poly (3,4-ethylenedioxythiophene) has a special place within the field of organic electronics due to its outstanding conductivity, stability, and processability. Since PEDOT was first synthesized in the late 1980s, a massive amount of knowledge has been accumulated about its morphological, structural, electrical, and optical properties, along with its applications in various devices. Notably, however, is that the vast majority of the reports in the field are purely experimental, without any theoretical support from simulation and modeling. In many other fields of material science, molecular modeling has already become a standard tool for guiding the experimental work. For PEDOT, the lack of the theoretical understanding of many important aspects of the material properties and device functionality leads to misconceptions and controversial issues hindering the progress in the field. The purpose of this Perspective is to fill the knowledge gaps and to present the current state-of-the art of the theoretical understanding of PEDOT. As theoretical understanding is essential to correctly interpretate experimental results and for the design of materials and devices with better performance, this Perspective targets equally experimental and theoretical communities working on PEDOT and related materials. We also hope that this Perspective will attract further attention of the computational community, which would help to bring the theoretical understanding of PEDOT to the levels already achieved in many other fields of material science.

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“… 23 Note that the Tafel slopes close to 40 mV/decade are also reported for platinum-based electrodes, 20 inorganic platinum-free catalysts, 24 and conducting polymers. 25 The wide range of Tafel slopes observed for the HER on the carbonous materials suggests a significant effect of the state of the surface. The higher electronic density of states (DOS) at the edge plane in comparison with the basal plane of graphene as the simplest level of structural organization of all graphitic materials results in a few orders-of-magnitude higher rates of the electron transfer observed on edges determining chemical and electrochemical anisotropy.…”

Section: Resultsmentioning

confidence: 99%

Bidirectional Hydrogen Electrocatalysis on Epitaxial Graphene

et al. 2022

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The climate change due to human activities stimulates the research on new energy resources. Hydrogen has attracted interest as a green carrier of high energy density. The sustainable production of hydrogen is achievable only by water electrolysis based on the hydrogen evolution reaction (HER). Graphitic materials are widely utilized in this technology in the role of conductive catalyst supports. Herein, by performing dynamic and steady-state electrochemical measurements in acidic and alkaline media, we investigated the bidirectional electrocatalysis of the HER and hydrogen oxidation reaction (HOR) on metal- and defect-free epigraphene (EG) grown on 4H silicon carbide (4H-SiC) as a ground level of structural organization of general graphitic materials. The absence of any signal degradation illustrates the high stability of EG. The experimental and theoretical investigations yield the coherent conclusion on the dominant HER pathway following the Volmer–Tafel mechanism. We ascribe the observed reactivity of EG to its interaction with the underlying SiC substrate that induces strain and electronic doping. The computed high activation energy for breaking the O–H bond is linked to the high negative overpotential of the HER. The estimated exchange current of HER/HOR on EG can be used in the evaluation of complex electrocatalytic systems based on graphite as a conducing support.

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Electrochemical hydrogen production on a metal-free polymer

Abstract: Demonstration of hydrogen production on metal-free poly(3,4-ethylenedioxythiophene (PEDOT) film.

Cited by 26 publications

References 68 publications

Faradaic Pixels for Precise Hydrogen Peroxide Delivery to Control M‐Type Voltage‐Gated Potassium Channels

Faradaic Pixels for Precise Hydrogen Peroxide Delivery to Control M‐Type Voltage‐Gated Potassium Channels

Electronic, Optical, Morphological, Transport, and Electrochemical Properties of PEDOT: A Theoretical Perspective

Bidirectional Hydrogen Electrocatalysis on Epitaxial Graphene

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