Mesoporous Hollow Carbon Sphere-Embedded MXene Architectures Decorated with Ultrafine Rh Nanocrystals toward Methanol Electrooxidation.

The development of advanced Pt-alternative anode electrocatalysts with high activity and reliable stability is critical to overcoming the technical challenges of direct methanol fuel cells. Here, we propose a robust bottom-up strategy for the spatial construction of mesoporous hollow carbon sphere (HCS)-embedded MXene architectures decorated with ultrafine Rh nanocrystals (Rh/HCS-MX) via stereoscopic coassembly reactions. The rational intercalation of HCS effectively separates the MXene nanowalls to achieve a rapid mass-transfer efficiency, while the intimate coupling of the hybrid carrier with Rh nanocrystals enables their electronic structure optimization, thus contributing to strong synergistic catalytic effects. Accordingly, the resulting Rh/HCS-MX architectures exhibit outstanding methanol electrooxidation properties in terms of large electrochemical active surface areas, high mass/specific activities, and good long-term stability, all of which are significantly superior to the traditional Rh/carbon black, Rh/HCS, and Rh/MXene as well as commercial Pt/carbon balck and Pd/carbon balck electrocatalysts.