In Situ Generated Dual-Template Method for Fe/N/S Co-Doped Hierarchically Porous Honeycomb Carbon for High-Performance Oxygen Reduction
In Situ Generated Dual-Template Method for Fe/N/S Co-Doped Hierarchically Porous Honeycomb Carbon for High-Performance Oxygen Reduction
复制标题
原位生成双模板方法用于 Fe/N/S 共掺杂分级多孔蜂窝碳的高性能氧还原
DOI：
10.1021/acsami.7b19645
复制
发表时间：
2018
影响因子：
9.5
通讯作者：
Chen Shengli
中科院分区：
文献类型：
--
作者：
Zeng Hongju;Wang Wang;Li Jun;Luo Jin;Chen Shengli
杂原子掺杂能够在碳材料中产生氧还原反应（ORR）的催化位点；而分级多孔结构对于此类活性炭催化剂中通常有限的催化位点的有效暴露和可及性是必要的。这项工作报道了一种原位生成的双模板方法来合成Fe/N/S共掺杂分级多孔碳（FeNS/HPC），以前体冻干过程中形成的NaCl微晶作为主要模板，生成具有超薄石墨烯碳层壁的~500 nm大孔，并在冷冻干燥过程中形成Fe3O4纳米颗粒。 采用高温碳化工艺作为二次模板，在大孔壁上产生中孔。除了有利于ORR的石墨-N、吡啶-N和噻吩-S共存外，所制备的FeNS/HPC还具有高度石墨化和互连的分级多孔结构，比表面积高达938 m2g-1。因此，它在碱性和酸性电解质中均表现出优异的四电子氧还原性能。原位生成和容易的溶液去除使得本模板方法成为大规模制备各种应用的活性多孔碳材料的有前途的方法。
Heteroatoms doping is able to produce catalytic sites in carbon materials for oxygen reduction reaction (ORR); while hierarchically porous structure is necessary for efficient exposure and accessibility of the usually limited catalytic sites in such activated carbon catalysts. This work reports an in situ generated dual-template method to synthesize the Fe/N/S co-doped hierarchically porous carbon (FeNS/HPC), with NaCl crystallites formed during the precursor lyophilization process as the primary template to generate ∼500 nm macropores with ultrathin graphene-like carbon-layer walls, and Fe3O4nanoparticles formed during the high-temperature carbonization process as the secondary template to produce mesopores on the walls of macropores. As well as the coexistence of graphitic-N, pyridinic-N, and thiophene-S which are beneficial to ORR, the as prepared FeNS/HPC possesses a highly graphitized and interconnected hierarchical porous structure, giving a specific surface area as high as 938 m2g–1. As a consequence, it exhibits excellent four-electron oxygen reduction performance in both alkaline and acid electrolytes. The in situ generation and facile solution removal make the present template method a promising way for scale-up preparation of active porous carbon materials for various applications.