Publications by authors named "Nemanja Danilovic"

Clean hydrogen production requires large-scale deployment of water-electrolysis technologies, particularly proton-exchange-membrane water electrolyzers (PEMWEs). However, as iridium-based electrocatalysts remain the only practical option for PEMWEs, their low abundance will become a bottleneck for a sustainable hydrogen economy. Herein, we propose high-performing and durable ionomer-free porous transport electrodes (PTEs) with facile recycling features enabling Ir thrifting and reclamation.

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Interfacial and bulk properties between the catalyst layer and the porous transport layer (PTL) restrict the iridium loading reduction for proton exchange membrane water electrolyzers (PEMWEs), by limiting their mass and charge transport. Using titanium fiber PTLs of varying thickness and porosity, the bulk and interface transport properties are investigated, correlating them to PEMWEs cell performance at ultra-low Ir loadings of ≈0.05 mg cm .

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Understanding the relationships between porous transport layer (PTL) morphology and oxygen removal is essential to improve the polymer electrolyte water electrolyzer (PEWE) performance. X-ray computed tomography and machine learning were performed on a model electrolyzer at different water flow rates and current densities to determine how these operating conditions alter oxygen transport in the PTLs. We report a direct observation of oxygen taking preferential pathways through the PTL, regardless of the water flow rate or current density (1-4 A/cm).

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We present ultralow Ir-loaded (ULL) proton exchange membrane water electrolyzer (PEMWE) cells that can produce enough hydrogen to largely decarbonize the global natural gas, transportation, and electrical storage sectors by 2050, using only half of the annual global Ir production for PEMWE deployment. This represents a significant improvement in PEMWE's global potential, enabled by careful control of the anode catalyst layer (CL), including its mesostructure and catalyst dispersion. Using commercially relevant membranes (Nafion 117), cell materials, electrocatalysts, and fabrication techniques, we achieve at peak a 250× improvement in Ir mass activity over commercial PEMWEs.

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We demonstrate the translation of a low-cost, non-precious metal cobalt phosphide (CoP) catalyst from 1 cm lab-scale experiments to a commercial-scale 86 cm polymer electrolyte membrane (PEM) electrolyser. A two-step bulk synthesis was adopted to produce CoP on a high-surface-area carbon support that was readily integrated into an industrial PEM electrolyser fabrication process. The performance of the CoP was compared head to head with a platinum-based PEM under the same operating conditions (400 psi, 50 °C).

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Hydrogen is an important part of any discussion on sustainability and reduction in emissions across major energy sectors. In addition to being a feedstock and process gas for many industrial processes, hydrogen is emerging as a fuel alternative for transportation applications. Renewable sources of hydrogen are therefore required to increase in capacity.

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The selection of oxide materials for catalyzing the oxygen evolution reaction in acid-based electrolyzers must be guided by the proper balance between activity, stability and conductivity-a challenging mission of great importance for delivering affordable and environmentally friendly hydrogen. Here we report that the highly conductive nanoporous architecture of an iridium oxide shell on a metallic iridium core, formed through the fast dealloying of osmium from an IrOs alloy, exhibits an exceptional balance between oxygen evolution activity and stability as quantified by the activity-stability factor. On the basis of this metric, the nanoporous Ir/IrO morphology of dealloyed IrOs shows a factor of ~30 improvement in activity-stability factor relative to conventional iridium-based oxide materials, and an ~8 times improvement over dealloyed IrOs nanoparticles due to optimized stability and conductivity, respectively.

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The growing need to store increasing amounts of renewable energy has recently triggered substantial R&D efforts towards efficient and stable water electrolysis technologies. The oxygen evolution reaction (OER) occurring at the electrolyser anode is central to the development of a clean, reliable and emission-free hydrogen economy. The development of robust and highly active anode materials for OER is therefore a great challenge and has been the main focus of research.

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Three of the fundamental catalytic limitations that have plagued the electrochemical production of hydrogen for decades still remain: low efficiency, short lifetime of catalysts and a lack of low-cost materials. Here, we address these three challenges by establishing and exploring an intimate functional link between the reactivity and stability of crystalline (CoS2 and MoS2) and amorphous (CoSx and MoSx) hydrogen evolution catalysts. We propose that Co(2+) and Mo(4+) centres promote the initial discharge of water (alkaline solutions) or hydronium ions (acid solutions).

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In the present study, we used a surface-science approach to establish a functional link between activity and stability of monometallic oxides during the OER in acidic media. We found that the most active oxides (Au ≪ Pt < Ir < Ru ≪ Os) are, in fact, the least stable (Au ≫ Pt > Ir > Ru ≫ Os) materials. We suggest that the relationships between stability and activity are controlled by both the nobility of oxides as well as by the density of surface defects.

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Understanding the functional links between the stability and reactivity of oxide materials during the oxygen evolution reaction (OER) is one key to enabling a vibrant hydrogen economy capable of competing with fossil fuel-based technologies. In this work, by focusing on the surface chemistry of monometallic Ru oxide in acidic and alkaline environments, we found that the kinetics of the OER are almost entirely controlled by the stability of the Ru surface atoms. The same activity-stability relationship was found for more complex, polycrystalline and single-crystalline SrRuO(3) thin films in alkaline solutions.

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The methods used to improve catalytic activity are well-established, however elucidating the factors that simultaneously control activity and stability is still lacking, especially for oxygen evolution reaction (OER) catalysts. Here, by studying fundamental links between the activity and stability of well-characterized monometallic and bimetallic oxides, we found that there is generally an inverse relationship between activity and stability. To overcome this limitation, we developed a new synthesis strategy that is based on tuning the near-surface composition of Ru and Ir elements by surface segregation, thereby resulting in the formation of a nanosegregated domain that balances the stability and activity of surface atoms.

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In developing cost-effective complex oxide materials for the oxygen evolution reaction, it is critical to establish the missing links between structure and function at the atomic level. The fundamental and practical implications of the relationship on any oxide surface are prerequisite to the design of new stable and active materials. Here we report an intimate relationship between the stability and reactivity of oxide catalysts in exploring the reaction on strontium ruthenate single-crystal thin films in alkaline environments.

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The development of hydrogen-based energy sources as viable alternatives to fossil-fuel technologies has revolutionized clean energy production using fuel cells. However, to date, the slow rate of the hydrogen oxidation reaction (HOR) in alkaline environments has hindered advances in alkaline fuel cell systems. Here, we address this by studying the trends in the activity of the HOR in alkaline environments.

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A novel, integral, tri-layered, proton conducting membrane SOFC was readily fabricated for simultaneous conversion of ethane at 650-700 degrees C to electrical power and ethylene with high selectivity.

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