Resilient High Catalytic Performance of Platinum Nanocatalysts with Porous Graphene Envelope.

Despite the innumerable developments of nanosized and well dispersed noble metal catalysts, the degradation of metal nanoparticle catalysts has proven to be a significant obstacle for the commercialization of the hydrogen fuel cell. Here, the formation of Pt nanoparticle catalysts with a porous graphene envelope has been achieved using a single step low temperature vaporization process. While these Pt-Gr core-shell nanoparticles possess superior resilience to degradation, it comes at the cost of degraded overall catalyst efficacy. However, it is possible to combat this lower overall performance through inclusion of low concentrations of nitrogen precursor in the initial stage of single-step synthesis, inhibiting the formation of complete graphene shells, as verified by atomic resolution aberration-corrected transmission electron microscopy (AC-TEM) imaging. The resultant porous graphene encapsulated Pt catalysts are found to have both the high peak performance of the bare Pt nanoparticle catalysts and the increased resilience of the fully shielded Pt-Gr core-shells, with the optimal N-doped Pt-Gr yielding a peak efficiency of 87% compared to bare Pt, and maintaining 90% of its catalytic activity after extended potential cycling. The nitrogen treated Pt-Gr core-shells thus act as an effective substitute catalyst for conventional bare Pt nanoparticles, maintaining their catalytic performance over prolonged use.