Hierarchical nitrogen-doped carbon nanocages （hNCNC） with large specific surface areas were used as a catalyst support to immobilize Pt nanoparticles by a microwave-assisted polyol method. The Pt/hNCNC catalyst with 20 wt% loading has a homogeneous dispersion of Pt nanoparticles with the average size of 3.3 nm, which is smaller than 4.3 and 4.9 nm for the control catalysts with the same loading supported on hierarchical carbon nanocages （hCNC） and commercial Vulcan XC-72, respec- tively. Accordingly, Pt/hNCNC has a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibited excellent electrocatalytic activity and stability for methanol oxidation, which was better than the control catalysts. This was attributed to the en- hanced interaction between Pt and hNCNC due to nitrogen participation in the anchoring function. By making use of the unique advantages of the hNCNC support, a heavy Pt loading up to 60 wt% was prepared without serious agglomeration, which gave a high peak-current density per unit mass of catalyst of 95.6 mA/mg for achieving a high power density. These results showed the potential of the Pt/hNCNC catalyst for methanol oxidation and of the new hNCNC support for wide applications.
将含氮聚合物聚苯胺(PANI)均匀地担载到具有大比表面积、多级孔结构和高导电性的3D碳纳米笼(CNC)表面,再热解PANI制得了N掺杂位富集于表面、且具有优良导电性的碳基纳米材料.通过改变热解温度和前驱物中PANI的含量,对热解产物的表面N含量和导电性进行了调控.优化得到的NCNC-2-900催化剂具有优异的氧还原反应(ORR)催化性能,其起始电位高(-46 m V vs Ag/Ag Cl),明显优于体相N掺杂的CNC(-105 m V),且稳定性好(运行10 h后仍保留96%活性).该结果表明在保持良好导电性的同时增加表面N掺杂位是提高碳基材料ORR活性的有效途径.
