2025 AIChE Annual Meeting

(189j) Atomically Dispersed Electrocatalysts in Porous Architecture for Fuel Cells and Water Electrolysis

Author

Jinwoo Lee - Presenter, Pohang University of Science and Technology
Single-atom catalysts (SACs) and atomically dispersed catalysts have attracted growing attention because the number of active sites, with unpredictable catalytic activity can be maximized. We have designed highly stable and high-loading atomically dispersed catalysts in porous architectures. We synthesized Ru SAC supported on WC1-x (Ru SA/WC1-x) for alkaline HOR reaction by an in situ high-temperature annealing strategy to induce strong interactions between Ru SA and the WC1-x support without forming of impurities (e.g., WOx) on the surface during the carburization, resulting in high Ru SA loading of up to 6.1 wt%. Despite the promise of Fe-N-Cs electrocatalysts as alternatives to expensive Pt, their oxygen reduction reaction (ORR) performance falls short. To address this, two carbon support-structural engineering methods were devised. Firstly, defect adjustment in ZIF-NC carbon support, derived from zeolitic imidazolate frameworks, via CO2 activation. Secondly, introduction of mesopores into ZIF-NC using the block co-polymer soft-template method. Controlled degree of defect sites in supports enhance intrinsic activity of Fe-N4 by modifying electronic structure such as charge distribution and spin state. Mesopores aid mass transport, improving active site accessibility. Additionally, the curved surfaces and carbon edge sites generated by mesopores alter the geometric structure of Fe-N4, optimizing the adsorption energy of oxygen species. Support-structural engineered Fe-N-Cs electrocatalysts exhibit relatively outstanding ORR performance compared to pristine Fe-N-C. MEAs with these electrocatalysts exhibit impressive peak power densities, highlighting their high activity at the MEA level. We also report self-assembly-assisted dynamic placement of noble metals selectively on multifunctional carbide supports for alkaline hydrogen electrocatalysts.