Hierarchical Wrinkle-Structured Catalyst Layer/Membrane Interface for Ultralow Pt-Loading Polymer Electrolyte Membrane Fuel Cells (PEMFCs).

The optimal architecture of three-dimensional (3D) interface between a polymer electrolyte membrane (PEM) and catalyst layer (CL) is one of the most important issues to improve PEM fuel cells' (PEMFCs) performance. Here, we report the fabrication of hierarchical wrinkled PEM/CL interface over a large area. We fabricated the hierarchical wrinkles on a multiscale from nanometers to micrometers by bottom-up-based facile, scalable, and simple method. Notably, it allows one to go beyond the limit of the catalyst utilization by extremely enlarged interfacial area. The resulting hierarchical wrinkled PEM/CL displays a dramatically increased electrochemically active surface area (ECSA) and power performance by the enhancement factors of 89% and 67% compared with those of flat interface, which is one of the best enhancements compared to previous PEMFCs. We believe the scalability of hierarchical wrinkled interface can be exploited to design advanced 3D interfaces for high-performance PEMFCs even with ultralow Pt-loading.

Catalytic production of impurity-free V3.5+ electrolyte for vanadium redox flow batteries.

The vanadium redox flow battery is considered one of the most promising candidates for use in large-scale energy storage systems. However, its commercialization has been hindered due to the high manufacturing cost of the vanadium electrolyte, which is currently prepared using a costly electrolysis method with limited productivity. In this work, we present a simpler method for chemical production of impurity-free V3.5+ electrolyte by utilizing formic acid as a reducing agent and Pt/C as a catalyst. With the catalytic reduction of V4+ electrolyte, a high quality V3.5+ electrolyte was successfully produced and excellent cell performance was achieved. Based on the result, a prototype catalytic reactor employing Pt/C-decorated carbon felt was designed, and high-speed, continuous production of V3.5+ electrolyte in this manner was demonstrated with the reactor. This invention offers a simple but practical strategy to reduce the production cost of V3.5+ electrolyte while retaining quality that is adequate for high-performance operations.

Achieving three-dimensional lithium sulfide growth in lithium-sulfur batteries using high-donor-number anions.

Uncontrolled growth of insulating lithium sulfide leads to passivation of sulfur cathodes, which limits high sulfur utilization in lithium-sulfur batteries. Sulfur utilization can be augmented in electrolytes based on solvents with high Gutmann Donor Number; however, violent lithium metal corrosion is a drawback. Here we report that particulate lithium sulfide growth can be achieved using a salt anion with a high donor number, such as bromide or triflate. The use of bromide leads to ~95 % sulfur utilization by suppressing electrode passivation. More importantly, the electrolytes with high-donor-number salt anions are notably compatible with lithium metal electrodes. The approach enables a high sulfur-loaded cell with areal capacity higher than 4 mA h cm-2 and high sulfur utilization ( > 90 %). This work offers a simple but practical strategy to modulate lithium sulfide growth, while conserving stability for high-performance lithium-sulfur batteries.

Tuning the Ionomer Distribution in the Fuel Cell Catalyst Layer with Scaling the Ionomer Aggregate Size in Dispersion.

With the demands for better performance of polymer electrolyte membrane fuel cells, studies on controlling the distribution of ionomers have recently gained interest. Here, we present a tunable ionomer distribution in the catalyst layer (CL) with dipropylene glycol (DPG) and water mixtures as the ionomer dispersion medium. Dynamic light scattering and molecular dynamics simulation demonstrate that, by increasing the DPG content in the dispersion, the size of the ionomer aggregates in the dispersion is exponentially reduced because of the higher affinity of DPG for Nafion ionomers. The ionomer distribution of the resulting CLs dictates the dimensional feature of the ionomer dispersion. Although the ionomer distribution becomes more uniform with increasing the DPG content, an optimal power performance is obtained at a DPG content of 50 wt % regardless of feed humidity because of balanced proton and mass transports. As a guide for tuning the ionomer distribution, we suggest that the ionomer aggregates in the dispersion with a size close to that of the Pt/C aggregates form a highly connected ionomer network and maintain a porosity in the catalyst/ionomer aggregate, resulting in high power performance.

In-Plane Channel-Structured Catalyst Layer for Polymer Electrolyte Membrane Fuel Cells.

In this study, we present a novel catalyst layer (CL) with in-plane flow channels to enhance the mass transports in polymer electrolyte membrane fuel cells. The CL with in-plane channels on its surface is fabricated by coating a CL slurry onto a surface-treated substrate with the inverse line pattern and transferring the dried CL from the substrate to a membrane. The membrane electrode assembly with the in-plane channel-patterned CL has superior power performances in high current densities compared with an unpatterned, flat CL, demonstrating a significant enhancement of the mass-transport property by the in-plane channels carved in the CL. The performance gain is more pronounced when the channel direction is perpendicular to the flow field direction, indicating that the in-plane channels increase the utilization of the CL under the rib area. An oxygen-transport resistance analysis shows that both molecular and Knudsen diffusion can be facilitated with the introduction of the in-plane channels. The direct CL patterning technique provides a platform for the fabrication of advanced CL structures with a high structural fidelity and design flexibility and a rational guideline for designing high-performance CLs.

Three-Dimensional Interlocking Interface: Mechanical Nanofastener for High Interfacial Robustness of Polymer Electrolyte Membrane Fuel Cells.

A scalable nanofastener featuring a 3D interlocked interfacial structure between the hydrocarbon membrane and perfluorinated sulfonic acid based catalyst layer is presented to overcome the interfacial issue of hydrocarbon membrane based polymer electrolyte membrane fuel cells. The nanofastener-introduced membrane electrode assembly (MEA) withstands more than 3000 humidity cycles, which is 20 times higher durability than that of MEA without nanofastener.