Due to the sluggish kinetics of the hydrogen oxidation reaction (HOR) in alkaline electrolytes, the development of more efficient HOR catalysts is essential for the next generation of anion‐exchange membrane fuel cells (AEMFCs). In this work, CeOx is selectively deposited onto carbon‐supported Pd nanoparticles by controlled surface reactions, aiming to enhance the homogenous distribution of CeOx and its preferential attachment to Pd nanoparticles, to achieve highly active CeOx‐Pd/C catalysts. The catalysts are characterized by inductively coupled plasma–atomic emission spectroscopy, X‐ray diffraction, high‐resolution transmission electron microscopy, scanning transmission electron microscopy (STEM), electron energy loss spectroscopy, and X‐ray photoelectron spectroscopy to confirm the bulk composition, phases present, morphology, elemental mapping, local oxidation, and surface chemical states, respectively. The intimate contact between Pd and CeOx is shown through high‐resolution STEM maps. The oxophilic nature of CeOx and its effect on Pd are probed by CO stripping. The interfacial contact area between CeOx and Pd nanoparticles is calculated for the first time and correlated to the electrochemical performance of the CeOx‐Pd/C catalysts. Highest recorded HOR specific exchange current (51.5 mA mg−1Pd) and H2–O2 AEMFC performance (peak power density of 1,169 mW cm−2 mgPd−1) are obtained with a CeOx‐Pd/C catalyst with Ce0.38/Pd bulk atomic ratio.

As polymer electrolyte membrane fuel cell technologies see increased use in the transportation and energy sectors, there continues to be a need to produce tunable, high-performance oxygen reduction reaction (ORR) catalysts. This work represents the first detailed investigation of commercially available mesoporous nitrogen-functionalized carbon supports with tunable properties (Engineered Carbon Supports, ECS) and ORR catalysts based on platinum nanoparticles (Pt-NPs) supported on these ECS materials produced by Pajarito Powders, LLC. The ECS materials with tunable concentrations of oxygen and nitrogen functional groups and varied carbon graphitization levels were investigated. First, the physicochemical properties of these Pt/ECS catalysts are presented, alongside their bare, Pt-free ECS analogue carbon support materials as investigated through a combination of characterization techniques. This yields a comprehensive catalog of physicochemical properties, including surface area, the concentration of surface dopants (nitrogen and oxygen), evaluation of graphitic content, morphology, and Pt-NP particle size distribution. Then, the ORR performance of the three different Pt/ECS catalysts in membrane electrode assemblies (MEAs) tested under low-relative-humidity conditions is presented as an example of the performance that can be obtained with these materials. All catalysts demonstrated very promising ORR performance at low relative humidity, achieving current densities between 1.8 and 1.3 A/cm2 at 0.6 V. This work demonstrates that carbon supports with engineered morphologies and compositions achieved through the VariPore synthetic technology developed by Pajarito Powders, LLC are a promising platform to produce supports and catalysts with tunable properties for a variety of applications.

We investigated the effect of platinum loading and layer thickness on cathode catalyst degradation by a comprehensive in-situ and scanning tunneling electron microscopy energy dispersive spectroscopy (STEM-EDS) characterization. To decouple the effect of platinum loading and layer thickness, the experiments were categorized in two sets, each with cathode loadings varying between 0.1 and 0.4 mgPt cm-2: (i) Samples with a constant Pt/C ratio and thus varying layer thickness, and (ii) samples with varying Pt/C ratios, achieved by dilution with bare carbon, to maintain a constant layer thickness at different platinum loadings. Every MEA was subjected to an accelerated stress test, where the cell was operated for 45,000 cycles between 0.6 and 0.95 V. Regardless of the Pt/C ratio, a higher relative loss in electrochemically active surface area was measured for lower Pt loadings. STEM-EDS measurements showed that Pt was mainly lost close to the cathode – membrane interface by the concentration driven Pt2+ ion flux into the membrane. The size of this Pt-depletion zone has shown to be independent on the overall Pt loading and layer thickness, hence causing higher relative Pt loss in low thickness electrodes, as the depletion zone accounts for a larger fraction of the catalyst layer

The maturity of the current polymer electrolyte membrane fuel cells (PEMFCs) has been product of the considerable scientific and industrial effort devoted to developing highly efficient and reliable versions of this technology, resulting in its increased application in the transportation and energy generation sectors. Fuel cells are one of the most advantageous solutions for clean energy applications due to their near-zero-emission, high efficiency, low maintenance cost, and high energy density. PEMFCs produce electricity through the electrochemical reaction of hydrogen and oxygen (or air) taking place in the Membrane Electrode Assembly (MEA) by converting chemical energy of the hydrogen oxidation and oxygen reduction into electrical energy with water as a byproduct. However, producing oxygen reduction reaction (ORR) catalysts with high performance at scale is still a challenge that needs to be tackled to enable an increment in energy generation of this technology. Additionally, tunability of the materials at the core of this technology is essential to meet the demands of the specific application and operating conditions. Here we investigate commercially available ORR catalysts based on platinum nanoparticles (Pt-NPs) supported on nitrogen-functionalized carbon (Engineered Carbon SupportsTM, ECSTM) produced by Pajarito Powder, LLC at scale. The ORR performance of three MEAs made with different Pt/ECS catalysts, by IRD Fuel Cells, LLC was studied under low relative humidity conditions, exhibiting competitive performance, and reaching current densities between 1.8 and 1.3 A/cm2 at 0.6 V, at extremely low loading of Pt – 0.1 mgPt cm-2. The physicochemical properties of these Pt/ECS catalysts alongside their Pt-free ECSTM analogue carbon support materials were comprehensively studied. For this purpose, several characterization techniques were used, such: X-ray diffraction, Raman spectroscopy, and transmission electron microscopy (TEM) to investigate structural and morphological properties, X-ray photoelectron spectroscopy to determine the surface composition and chemical properties, thermogravimetric analysis to evaluate thermal oxidation properties, and nitrogen sorption to determine the surface area and porosity, of the materials. This thorough characterization enabled us to determine that the best performing catalyst in the conditions used in this work have the highest surface area and the highest concentration of surface dopants (nitrogen and oxygen). Although, catalyst supported on lower surface area carbon, but with higher graphitic content, also exhibited competitive performance that can be exploited in applications where more corrosion-resistant carbon is needed. Finally, based on the highly competitive MEA performance for the three Pt/ECS catalysts supported on these carbons, our work demonstrates that these carbon supports (developed by Pajarito Powder, LLC) with engineered morphology and composition fabricated through VariPoreTM synthetic technology can result in tunable properties suitable for a targete...