Herein, we report energy storage devices, which are based on densely packed, vertically aligned MoS2 (VA-MoS2) or planar oriented MoS2 (PO-MoS2) and compare their electrochemical performances. The VA-MoS2 films have been processed by chemical vapor deposition (CVD) to reach unprecedented micron-scale thick films while maintaining the vertical alignment for the whole thickness. The VA-MoS2 and the PO-MoS2 films form a high-performance Li-ion electrode, reaching the theoretical limits of reversible capacity for this material (800 mAh/g; twice the specific capacity of graphite). The vertical alignment allows faster charge-discharge rates while maintaining a high specific capacity (C-rate measurements). Noteworthy, the reversible cycling of the Li-ion electrode also benefits from the vertical alignment. In this article, we present the full synthesis, structural and electrochemical characterization of VA-MoS2 along with the properties of PO-MoS2 to deconvolute the intrinsic properties of MoS2 from the influence of the layers’ orientation.

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Platinum is the most used electrocatalyst in proton exchange membrane fuel cells (PEMFCs). Nonetheless, it suffers from various types of degradation. Identical location electron microscopy has previously been used to observe local catalyst changes under accelerated stress tests (ASTs), giving insight into how individual catalyst particles degrade. However, it is important that such studies are carried out under relevant reaction conditions, as these can differ substantially between liquid half-cells and real PEMFC conditions. In this work, a single cell PEMFC was used to study the degradation of a commercial Pt-catalyzed membrane electrode assembly by performing square wave voltage ASTs in a potential range of 0.6 to 1.0 V. Identical location scanning electron microscopy (IL-SEM) was used to follow the degradation of the cathodic catalytic layer (CL) throughout 14,000 AST cycles. From the IL-SEM, we can conclude that the Pt nanoparticles degrade via Ostwald ripening, crystal migration, and coalescence. Small Pt nanoparticles agglomerate to larger particles or dissolve and redeposit to more stable particles, increasing the average particle size during the ASTs. In addition, cross-sectional TEM images show thinning of the ionomer layer during the AST procedure. The IL-SEM technique facilitates observation of local degradation of the CL in real PEMFCs, which will help to understand different degradation mechanisms, allowing for better solutions to be designed.

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The efficient formulation of silicon based, highloading electrode with good capacity retention and cycling stability remains challenging. To gain a better understanding of the ongoing processes and failure mechanisms occurring during battery performance, operando micro-Raman spectroscopy is helpful to map the active silicon sites. Herein, we present the investigation of the electrochemical performance of anodes composed of plasmonic metal (Ag and Au) decorated silicon, designed for enhancing Raman signal. Following the discovery that only a partial amount of the electroactive material undergoes lithiation in the first cycle, we show that the plasmonic metal tips can enhance the connectivity of the Si particles. The micro-Raman mapping of electroactive silicon material reveals how the plasmonic metals influence the distribution of silicon active sites during battery cycling. The ratio of electroactive Si is found to increase from Si to Si/Au and Si/Ag electrodes, and the results are explained in terms of interconnectivity of the particles.

The synthetic control through colloidal synthesis led to a remarkable increase in platinum mass activity in octahedral nanocrystals with Pt-rich surface. In this manuscript, we demonstrate that the ratio of...

PtNi is amongst the most active electrocatalyst for the oxygen reduction reaction, but its stability in operation is uncertain. Intuitively, alkaline environments lead to milder degradations than acidic ones, although carbon-supported Pt-group metal nanoparticles are particularly degraded even in dilute alkaline electrolytes. To date, PtNi catalysts durability has not been characterized for alkaline oxygen reduction and evolution reactions (ORR and OER). Herein, carbon-supported shape controlled PtNi catalysts were compared in terms of activity and durability during alkaline ORR and OER. The PtNi catalysts are shape-controlled Pt-rich alloy, Ni-rich alloy, and Pt core/Ni shell (Pt@Ni) synthesized on Vulcan XC72R carbon. Their morphology and composition were evaluated by identical-location transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray diffraction pre and post accelerated stress test. Compared to Pt/C and Ni/C benchmark catalysts, the core-shell and Nirich alloy catalysts gave high and stable OER activities. After accelerated stress test, the catalysts show two features which are believed to play a major role in the durability: a Ni-enrichment at the nanoparticles' surface and an improved attachment of the catalyst to the carbon support.

Platinum (Pt) is a widely used electrocatalyst material in fuel cells and electrolysers. Proton exchange membrane (PEM) fuel cells and electrolysis operate under highly acidic conditions whereas the more recently developed anion exchange membrane (AEM) processes take place under alkaline conditions. Pt dissolution and Pt oxidation during operation and varying potentials has been studied mainly for the acidic PEM and less for the alkaline AEM. This study presents a comparison of Pt dissolution and Pt oxidation in 0.5 M H2SO4 and 1 M KOH using electrochemical quartz crystal microbalance (EQCM) on Pt thin films. Physical characterisation using electron microscopy and atomic force microscopy (AFM) revealed small, yet significant differences in the Pt film surface structure, which is related to differences in measured electrochemical surface area (ECSA). The mass increase from adsorption of oxygenated species and Pt oxidation is higher in alkaline conditions compared to in acid while dissolution of Pt is similar.