Search

Polymer electrolyte membrane fuel cells (PEMFCs) have attracted much attention as highly efficient, eco-friendly energy conversion devices. However, carbon-supported Pt (Pt/C) catalysts for PEMFCs still have several problems, such as low long-term stability, to be widely commercialized in fuel cell applications. To address the stability issues of Pt/C such as the dissolution, detachment, and agglomeration of Pt nanoparticles under harsh operating conditions, we design an interesting fabrication process to produce a highly active and durable Pt catalyst by introducing a robust carbon shell on the Pt surface. Furthermore, this approach provides insights into how to regulate the carbon shell layer for fuel cell applications. Through the application of an appropriate amount of H2 gas during heat treatment, the carbon shell pores, which are integral to the structure, can be systematically modulated to facilitate oxygen adsorption for the oxygen reduction reaction. Simultaneously, the carbon shell functions as a protective barrier, preventing catalyst degradation. In this regard, we investigate an in-depth analysis of the effects of critical parameters including H2 content and the flow rate of H2/N2 mixed gas during heat treatment to prepare better catalysts. [ABSTRACT FROM AUTHOR]

Proton exchange membrane fuel cells (PEMFCs) face technical issues of performance degradation due to catalyst dissolution and agglomeration in real-world operations. To address these challenges, intensive research has been recently conducted to introduce additional structural units on the catalyst surface. Among various concepts for surface modification, carbon shell encapsulation is known to be a promising strategy since the carbon shell can act as a protective layer for metal nanoparticles. As an interesting approach to form carbon shells on catalyst surfaces, the precursor ligand-induced formation is preferred due to its facile synthesis and tunable control over the carbon shell porosity. However, the origin of the carbon source and the carbon shell formation mechanism have not been studied in depth yet. Herein, this study aims to investigate carbon sources through the use of different precursors and the introduction of new methodologies related to the ligand exchange phenomenon. Subsequently, we provide new insights into the carbon shell formation mechanism using X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). Finally, the thermal stability and electrochemical durability of carbon shells are thoroughly investigated through in situ transmission electron microscopy (in situ TEM) and accelerated durability tests. [ABSTRACT FROM AUTHOR]

The performance of polymer electrolyte membrane fuel cells (PEMFCs) is deteriorated by the occurrence of reverse current flow. To suppress the reverse current flow, a hydrogen oxidation reaction (HOR)‐selective catalyst based on the molecular sieve effect should be developed. Here, considering the carbon solubility in transition metals, carbon shell‐encapsulated metal alloy nanoparticles with superior HOR selectivity were fabricated using carbon source in metal precursors. In particular, we introduced carbon solubility as the important parameter that should be considered in the catalyst design. Using Pt and Co with different carbon solubility, as a model catalyst, the effect of the metal composition of the core material on the carbon shell structure was discussed in detail. Due to the formation of high‐density carbon shell and Pt‐rich surface on the alloy nanoparticle, the HOR selectivity was remarkably enhanced. Therefore, this study provides insights into the development of carbon shell‐encapsulated nanoparticles for reaction‐selective catalysis. [ABSTRACT FROM AUTHOR]

[Display omitted] • Poisoning effect of benzene-containing hydrocarbon-based ionomers on Pt catalysts. • Two types of orientation-dependent adsorption of benzenesulfonic acid anion for Pt. • Changes in PZTC of Pt surface according to the sequence of electrolyte replacement. • Combination of various electrochemical analyses and XPS/TPD measurements. • Time-dependent anion adsorption affecting the long-term stability of fuel cell electrodes. Membrane electrode assembly (MEA) is an essential component that mainly determines the performance of proton exchange membrane fuel cells (PEMFCs). In the electrodes of the MEA, ionomers are mixed with Pt-based nanoparticles to transfer protons to the Pt surface where electrochemical reactions take place. However, Pt catalysts suffer from the poisoning effect of ionomers with proton-conducting groups such as sulfonic acid (SA), resulting in performance deterioration. In particular, for emerging hydrocarbon-based ionomers, the benzene group, which is commonly used to improve their chemical structure, accelerates the poisoning effect. Herein, we experimentally simulate the adsorption of SA and benzenesulfonic acid (BSA) on Pt nanoparticles, revealing the orientation-dependent poisoning effect of BSA on the Pt surface. [ABSTRACT FROM AUTHOR]