Yang Jing, Hübner René, Zhang Jiangwei, Wan Hao, Zheng Yuanyuan, Wang Honglei, Qi Haoyuan, He Lanqi, Li Yi, Dubale Amare Aregahegn, Sun Yujing, Liu Yuting, Peng Daoling, Meng Yuezhong, Zheng Zhikun, Rossmeisl Jan, Liu Wei
The Key Laboratory of Low-Carbon Chemistry & Energy Conservation of Guangdong Province, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, State Key Laboratory of Optoelectronic Materials and Technologies, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275, P. R. China.
Helmholtz-Zentrum Dresden-Rossendorf, Institute of Ion Beam Physics and Materials Research, Bautzner Landstrasse 400, 01328, Dresden, Germany.
Angew Chem Int Ed Engl. 2021 Apr 19;60(17):9590-9597. doi: 10.1002/anie.202015679. Epub 2021 Mar 17.
Insufficient catalytic activity and stability and high cost are the barriers for Pt-based electrocatalysts in wide practical applications. Herein, a hierarchically porous PtNi nanoframe/N-doped graphene aerogel (PtNiNF-NGA) electrocatalyst with outstanding performance toward methanol oxidation reaction (MOR) in acid electrolyte has been developed via facile tert-butanol-assisted structure reconfiguration. The ensemble of high-alloying-degree-modulated electronic structure and correspondingly the optimum MOR reaction pathway, the structure superiorities of hierarchical porosity, thin edges, Pt-rich corners, and the anchoring effect of the NGA, endow the PtNiNF-NGA with both prominent electrocatalytic activity and stability. The mass and specific activity (1647 mA mg , 3.8 mA cm ) of the PtNiNF-NGA are 5.8 and 7.8 times higher than those of commercial Pt/C. It exhibits exceptional stability under a 5-hour chronoamperometry test and 2200-cycle cyclic voltammetry scanning.
催化活性不足、稳定性差以及成本高昂是限制铂基电催化剂广泛实际应用的障碍。在此，通过简便的叔丁醇辅助结构重构方法，制备了一种对酸性电解质中的甲醇氧化反应（MOR）具有优异性能的分级多孔PtNi纳米框架/N掺杂石墨烯气凝胶（PtNiNF-NGA）电催化剂。高合金化程度调制的电子结构组合以及相应的最佳MOR反应路径、分级孔隙率、薄边缘、富铂角的结构优势以及NGA的锚定效应，赋予了PtNiNF-NGA突出的电催化活性和稳定性。PtNiNF-NGA的质量活性和比活性（分别为1647 mA mg 、3.8 mA cm ）比商业Pt/C高5.8倍和7.8倍。在5小时计时电流法测试和2200次循环伏安扫描下，它表现出卓越的稳定性。
