cell technologies has been hindered by a number of technical challenges, including the sluggish kinetics of the oxygen reduction reaction (ORR) at the cathode, [9][10][11][12][13][14] components' stability during long-term operation, [15,16] and the poisoning of the electrocatalyst with ethanol and CO fuels at the anode, e.g., as in the case of DMFCs. [17] Pt-based electrocatalysts with various compositions, facets, and morphologies have been explored to enhance the electrocatalytic activity towards the ORR. [18][19][20][21][22][23][24] In parallel, the development of catalyst support materials has also been critical in the overall development of Pt-based and other precious metal-based electrocatalysts and in the reduction of the metal catalyst loadings. Among the many support materials in use, carbon black Vulcan XC-72R (denoted as VC) has been reported to significantly improve the electrocatalytic activity towards the ORR of the supported Pt-based electrocatalysts and cell performance of PEMFCs, and is, therefore, a widely used support material for the commercial Pt-based electrocatalysts. [25][26][27][28] Among supported Pt-based electrocatalysts, carbon-supported Pt nanoparticles (NPs) are the most frequently investigated, [29,30] and one example is the commercial Pt(20 wt%)NPs/VC (Johnson Matthey) which represents the state-of-the-art electrocatalyst for low-temperature fuel cell applications. [1][2][3] Although this catalyst has demonstrated high activities in many electrocatalytic applications, its stability deteriorates during long-term electrochemical operation and this mainly results from the corrosion of the support material (i.e., VC) and the agglomeration or loss of the supported Pt NPs. When higher Pt contents (i.e., 40 or 60 wt%) are used in the catalyst layer, the stability is exacerbated because the Pt NPs in these high Pt content catalysts have a larger grain size than the Pt(20 wt%)NPs/VC catalyst, resulting in an uneven distribution and agglomeration. [1] Therefore, it is particularly important to modify VC-supported Pt-based catalysts for improved durability.To improve the long-term electrochemical stability of supported Pt-based electrocatalysts, various strategies have been developed, including the use of modified carbon support materials, [16] non-carbon catalyst supports, [15] a core-protected platinum monolayer shell, [14] and coplanar Pt/C nanomeshes, [13] etc. In addition, an ultrathin N-doped carbon shell formed in situ on PtFe NPs has been shown to be effective in Carbon-supported Pt-based electrocatalysts have been widely investigated for diverse electrochemical energy storage and conversion applications. Vulcan XC72R (VC) supported Pt(20 wt%) nanoparticles (NPs) (denoted as Pt(20 wt%)NPs/VC produced by Johnson Matthey (JM)) is the most commonly-used catalyst and is thus widely considered to be the state-of-theart electrocatalyst. Although Pt(20 wt%)NPs/VC(JM) has demonstrated very good electrocatalytic performance in these applications, further improvement in its electrocatalytic a...