Structural engineering carbon support in controlling the dopant concentrations or types and their homogeneity is an effective way to modulate the catalytic properties of Pt-based materials. Herein, we reported a convenient and scalable strategy to incorporate pyridinic and pyrrolic N components into the carbon matrix via quantum dots anchoring pathway. The newly designed carbon can accurately regulate the N contents, and importantly, exposes numerous functional edge sites for growing and stabilizing Pt nanoparticles with a very narrow size distribution. Experimental validation identified that a strengthened metal-support interaction is afforded on this Pt/NCB-n architecture, which significantly optimizes its catalytic behaviors toward the methanol electrooxidation process. Combining its unique textural features including unimpeded electron conductivity, intensive N components on the triple-phase boundaries, and sufficient accessible catalytically active centers, the obtained Pt/NCB-n exhibits a marvelous electrocatalytic activity accompanied by distinguished antipoisoning ability and reliable long-term stability, holding great potential as substitutes for conventional Pt-activated carbon catalysts. This study paves a new avenue to develop more effective carbon-based supports for constructing advanced electrocatalysts and can also be extended to the next-generation metal-air batteries, metal-ion batteries, or sensors.

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