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1.
Artículo en Inglés | MEDLINE | ID: mdl-39293816

RESUMEN

The enhanced utilization of noble metal catalysts through highly porous nanostructures is crucial to advancing the commercialization prospects of proton exchange membrane water electrolysis (PEMWE). In this study, hierarchically structured IrOx-based nanofiber catalyst materials for acidic water electrolysis are synthesized by electrospinning, a process known for its scalability and ease of operation. A calcination study at various temperatures from 400 to 800 °C is employed to find the best candidates for both electrocatalytic activity and stability. Morphology, structure, phase, and chemical composition are investigated using a scale-bridging approach by SEM, TEM, XRD, and XPS to shed light on the structure-function relationship of the thermally prepared nanofibers. Activity and stability are monitored by a scanning flow cell (SFC) coupled with an inductively coupled plasma mass spectrometer (ICP-MS). We evaluate the dissolution of all metals potentially incorporated into the final catalyst material throughout the synthesis pathway. Despite the opposite trend of performance and stability, the present study demonstrates that an optimum between these two aspects can be achieved at 600 °C, exhibiting values that are 1.4 and 2.4 times higher than those of the commercial reference material, respectively. The dissolution of metal contaminations such as Ni, Fe, and Cr remains minimal, exhibiting no correlation with the steps of the electrochemical protocol applied, thus exerting a negligible influence on the stability of the nanofibrous catalyst materials. This work demonstrates the scalability of electrospinning to produce nanofibers with enhanced catalyst utilization and their testing by SFC-ICP-MS. Moreover, it illustrates the influence of calcination temperature on the structure and chemical composition of the nanofibers, resulting in outstanding electrocatalytic performance and stability compared to commercial catalyst materials for PEMWE.

2.
J Am Chem Soc ; 145(30): 16517-16525, 2023 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-37467341

RESUMEN

High-throughput synthesis of solution-processable structurally variable small-molecule semiconductors is both an opportunity and a challenge. A large number of diverse molecules provide a possibility for quick material discovery and machine learning based on experimental data. However, the diversity of the molecular structure leads to the complexity of molecular properties, such as solubility, polarity, and crystallinity, which poses great challenges to solution processing and purification. Here, we first report an integrated system for the high-throughput synthesis, purification, and characterization of molecules with a large variety. Based on the principle "Like dissolves like," we combine theoretical calculations and a robotic platform to accelerate the purification of those molecules. With this platform, a material library containing 125 molecules and their optical-electronic properties was built within a timeframe of weeks. More importantly, the high repeatability of recrystallization we design is a reliable approach to further upgrading and industrial production.

3.
J Am Chem Soc ; 145(11): 6398-6409, 2023 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-36892000

RESUMEN

The oxygen evolution reaction (OER) is crucial to future energy systems based on water electrolysis. Iridium oxides are promising catalysts due to their resistance to corrosion under acidic and oxidizing conditions. Highly active iridium (oxy)hydroxides prepared using alkali metal bases transform into low activity rutile IrO2 at elevated temperatures (>350 °C) during catalyst/electrode preparation. Depending on the residual amount of alkali metals, we now show that this transformation can result in either rutile IrO2 or nano-crystalline Li-intercalated IrOx. While the transition to rutile results in poor activity, the Li-intercalated IrOx has comparative activity and improved stability when compared to the highly active amorphous material despite being treated at 500 °C. This highly active nanocrystalline form of lithium iridate could be more resistant to industrial procedures to produce PEM membranes and provide a route to stabilize the high populations of redox active sites of amorphous iridium (oxy)hydroxides.

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