The development of active and durable proton exchange membrane fuel cell catalysts with high loading (ca. 40%) is critical for the commercialization of hydrogen fuel cells. Herein we report on the synthesis of a novel Pt/C catalyst using a novel bowl-like broken hollow carbon sphere (and N doped sphere) support (carbon shell thickness ~ 4.6 nm). Highly dispersed Pt nanoparticles (dPt ~ 4 nm) were deposited on both supports and within the carbon shell. The Pt particles in the pores were exposed on both sides of the shell, while the shell porosity ensured pore confinement of the Pt. Both catalysts exhibited high electrochemical surface areas (60-65 m 2 g -1 ) and cycling durability (6000 cycles) that was superior to a commercial benchmark Pt/C catalyst. These studies indicate that high loadings of confined small Pt particles on both sides of thin interconnected carbons can lead to high oxygen reduction reaction activities and durability.
The durability and long-term applicability of catalysts are critical parameters for the commercialization and adoption of fuel cells. Even though a few studies have been conducted on hollow carbon spheres (HCSs) as supports for Pt in oxygen reduction reactions (ORR) catalysis, in-depth durability studies have not been conducted thus far. In this study, Pt/HCSs and Pt/nitrogen-doped HCSs (Pt/NHCSs) were prepared using a reflux deposition technique. Small Pt particles were formed with deposition on the outside of the shell and inside the pores of the shell. The new catalysts demonstrated high activity (>380 μA cm−2 and 240 mA g−1) surpassing the commercial Pt/C by more than 10%. The catalysts demonstrated excellent durability compared to a commercial Pt/C in load cycling, experiencing less than 50% changes in the mass-specific activity (MA) and surface area-specific activity (SA). In stop-start durability cycling, the new materials demonstrated high stability with more than 50% retention of electrochemical active surface areas (ECSAs). The results can be rationalised by the high BET surface areas coupled with an array of meso and micropores that led to Pt confinement. Further, pair distribution function (PDF) analysis of the catalysts confirmed that the nitrogen and oxygen functional groups, as well as the shell curvature/roughness provided defects and nucleation sites for the deposition of the small Pt nanoparticles. The balance between graphitic and diamond-like carbon was critical for the electronic conductivity and to provide strong Pt-support anchoring.
The Cover Feature shows the cobalt oxide nanoparticles supported both inside and outside hollow carbon spheres (HCSs), which serve as a catalyst for benzyl alcohol oxidation. A metal oxidation step prior to the reaction enhanced the catalytic activity of benzyl alcohol which was used as a model reaction for the catalysts. Both catalysts showed similar activity and selectivity (to benzaldehyde) whether placed inside or outside the HCSs (70% selectivity at 50% conversion). No poisoning was observed due to product build up in the HCSs. More information can be found in the Full Paper by Pumza Mente et al.
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