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Overpotential

About: Overpotential is a research topic. Over the lifetime, 16474 publications have been published within this topic receiving 616632 citations.


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Journal ArticleDOI
TL;DR: The first example of in situ exfoliated, edge-rich, oxygen-functionalized graphene on the surface of carbon fibers using Ar plasma treatment is successfully prepared and has a higher specific surface area and an increased number of active sites for OER and ORR.
Abstract: Metal-free electrocatalysts have been extensively developed to replace noble metal Pt and RuO2 catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in fuel cells or metal-air batteries. These electrocatalysts are usually deposited on a 3D conductive support (e.g., carbon paper or carbon cloth (CC)) to facilitate mass and electron transport. For practical applications, it is desirable to create in situ catalysts on the carbon fiber support to simplify the fabrication process for catalytic electrodes. In this study, the first example of in situ exfoliated, edge-rich, oxygen-functionalized graphene on the surface of carbon fibers using Ar plasma treatment is successfully prepared. Compared to pristine CC, the plasma-etched carbon cloth (P-CC) has a higher specific surface area and an increased number of active sites for OER and ORR. P-CC also displays good intrinsic electron conductivity and excellent mass transport. Theoretical studies show that P-CC has a low overpotential that is comparable to Pt-based catalysts, as a result of both defects and oxygen doping. This study provides a simple and effective approach for producing highly active in situ catalysts on a carbon support for OER and ORR.

563 citations

Journal ArticleDOI
TL;DR: A cobalt-phthalocyanine-based high-performance carbon dioxide reduction electrocatalyst material developed with a combined nanoscale and molecular approach that exhibits >95% Faradaic efficiency for carbon monoxide production in a wide potential range and extraordinary catalytic activity.
Abstract: Electrochemical reduction of carbon dioxide with renewable energy is a sustainable way of producing carbon-neutral fuels. However, developing active, selective and stable electrocatalysts is challenging and entails material structure design and tailoring across a range of length scales. Here we report a cobalt-phthalocyanine-based high-performance carbon dioxide reduction electrocatalyst material developed with a combined nanoscale and molecular approach. On the nanoscale, cobalt phthalocyanine (CoPc) molecules are uniformly anchored on carbon nanotubes to afford substantially increased current density, improved selectivity for carbon monoxide, and enhanced durability. On the molecular level, the catalytic performance is further enhanced by introducing cyano groups to the CoPc molecule. The resulting hybrid catalyst exhibits >95% Faradaic efficiency for carbon monoxide production in a wide potential range and extraordinary catalytic activity with a current density of 15.0 mA cm−2 and a turnover frequency of 4.1 s−1 at the overpotential of 0.52 V in a near-neutral aqueous solution. Electrochemical reduction of carbon dioxide is a sustainable way of producing carbon-neutral fuels. Here, the authors take a combined nanoscale and molecular approach to develop a highly active and selective cobalt phthalocyanine/carbon nanotube hybrid electrocatalyst for carbon dioxide reduction to carbon monoxide.

563 citations

Journal ArticleDOI
TL;DR: A model based on density functional theory calculations is developed to describe trends in catalytic activity for CO2 electroreduction to CO in terms of the adsorption energy of the reaction intermediates, CO and COOH and shows that the strong scaling between adsorbed CO and adsorbates on metal surfaces is responsible for the persistent overpotential.
Abstract: We develop a model based on density functional theory calculations to describe trends in catalytic activity for CO2 electroreduction to CO in terms of the adsorption energy of the reaction intermediates, CO and COOH The model is applied to metal surfaces as well as the active site in the CODH enzymes and shows that the strong scaling between adsorbed CO and adsorbed COOH on metal surfaces is responsible for the persistent overpotential The active site of the CODH enzyme is not subject to these scaling relations and optimizes the relative binding energies of these adsorbates, allowing for an essentially reversible process with a low overpotential

563 citations

Journal ArticleDOI
TL;DR: In this article, a cobalt molybdenum phosphide nanocrystal coated by a few-layer N-doped carbon shell (CoMoP@C) is used for hydrogen evolution reaction.
Abstract: The hydrogen evolution reaction (HER) based on water electrolysis is a promising strategy for hydrogen energy production, in which the key point is seeking low-cost, high efficiency and stable electrocatalysts. Currently, the most efficient electrocatalysts for the HER are Pt-based catalysts (especially commercial Pt/C), but the low abundance and high cost of Pt hinder their widespread application. Herein, we demonstrate that a cobalt molybdenum phosphide nanocrystal coated by a few-layer N-doped carbon shell (CoMoP@C) is an excellent substitute for the HER. CoMoP@C is prepared by a one-step pyrolysis method on a large scale with polyoxometalate (POM) as a molecular platform. The catalytic activity of CoMoP@C is close to that of commercial 20% Pt/C under pH = 0–1 conditions and superior to that of 20% Pt/C under pH = 2–14 conditions at high overpotential (e.g. η > 240 mV at pH = 2.2). In real seawater, CoMoP@C exhibits stable HER performance with a high Faradaic efficiency (FE) of 92.5%, while the HER activity of 20% Pt/C dramatically decreases after 4 h. The remarkable HER performance of CoMoP@C should be attributed to the low free energy of H on the central CoMoP crystalline core and the multiple functions of the outer N-doped C shell (especially the strong H+ absorption behavior). This work may provide new options for the design and preparation of promising HER electrocatalysts superior to Pt/C, which can be used directly in seawater.

559 citations

Journal ArticleDOI
TL;DR: In this article, the authors reviewed the research progress in the development of carbon-based electrocatalysts toward hydrogen evolution reaction (HER) in acid electrolytes throughout the past few years.

559 citations


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Performance
Metrics
No. of papers in the topic in previous years
YearPapers
20232,316
20224,268
20212,838
20202,411
20192,174
20181,740