Approaching Industrially Relevant Current Densities for Hydrogen Oxidation with a Bioinspired Molecular Catalytic Material
- 22 October 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 143 (43), 18150-18158
- https://doi.org/10.1021/jacs.1c07093
Abstract
Integration of efficient platinum-group-metal (PGM)-free catalysts to fuel cells and electrolyzers is a prerequisite to their large-scale deployment. Here, we describe the development of a molecular-based anode for the hydrogen oxidation reaction (HOR) through noncovalent integration of a DuBois type Ni bioinspired molecular catalyst at the surface of a carbon nanotube modified gas diffusion layer. This mild immobilization strategy enabled us to gain high control over the loading in catalytic sites. Additionally, through the adjustment of the hydration level of the active layer, a new record current density of 214 ± 20 mA cm–2 could be reached at 0.4 V vs RHE with the PGM-free anode, at 25 °C. Near industrially relevant current densities were obtained at 55 °C with 150 ± 20 and 395 ± 30 mA cm–2 at 0.1 and 0.4 V overpotentials, respectively. These results further demonstrate the relevance of such molecular approaches for the development of electrocatalytic platforms for energy conversion.Keywords
Funding Information
- Agence Nationale de la Recherche (ANR-17-EURE-0003)
- Horizon 2020 Framework Programme
- Fuel Cells and Hydrogen Joint Undertaking (GAN 779366)
- Commissariat ?? l'??nergie Atomique et aux ??nergies Alternatives
This publication has 85 references indexed in Scilit:
- A Noble-Metal-Free Hydrogen Evolution Catalyst Grafted to Visible Light-Absorbing SemiconductorsThe Journal of Physical Chemistry Letters, 2013
- Electrochemistry, AFM, and PM-IRRA Spectroscopy of Immobilized Hydrogenase: Role of a Hydrophobic Helix in Enzyme Orientation for Efficient H2 OxidationAngewandte Chemie, 2011
- Hydrogenases as catalysts for fuel cells: Strategies for efficient immobilization at electrode interfacesElectrochimica Acta, 2011
- Low-platinum and platinum-free catalysts for the oxygen reduction reaction at fuel cell cathodesEnergy & Environmental Science, 2011
- Recent advances in non-precious metal catalysis for oxygen-reduction reaction in polymer electrolyte fuelcellsEnergy & Environmental Science, 2010
- Characterization and performances of cobalt–tungsten and molybdenum–tungsten carbides as anode catalyst for PEFCElectrochimica Acta, 2009
- Direct Electrochemistry of Redox Enzymes as a Tool for Mechanistic StudiesChemical Reviews, 2008
- Investigating and Exploiting the Electrocatalytic Properties of HydrogenasesChemical Reviews, 2007
- Tungsten and nickel tungsten carbides as anode electrocatalystsElectrochimica Acta, 2007
- Synthesis and characterization of high-surface area tungsten carbides and application to electrocatalytic hydrogen oxidationApplied Catalysis A: General, 2007