Self-assembly strategy for Co/N-doped meso/microporous carbon toward superior oxygen reduction catalysts
Self-assembly strategy for Co/N-doped meso/microporous carbon toward superior oxygen reduction catalysts
复制标题
DOI：
10.1016/j.colsurfa.2021.127395
复制
发表时间：
2021-08
期刊：
影响因子：
--
通讯作者：
Y. Shu;K. Ota;K. Miyake;Y. Uchida;S. Tanaka;N. Nishiyama
中科院分区：
文献类型：
--
作者：
Y. Shu;K. Ota;K. Miyake;Y. Uchida;S. Tanaka;N. Nishiyama
质子交换膜燃料电池（PEMFC）作为一种可持续、可再生、高效且环保的电化学能源转换系统而备受关注。作为阴极反应的缓慢的氧还原反应(ORR)是阻碍PEMFC实际使用的主要因素。当今ORR最有效的催化剂是铂基催化剂，其稀缺性高且对甲醇的耐久性低。因此，最近人们致力于探索过渡金属和杂原子掺杂碳材料在燃料电池中的大规模和商业应用。在此，我们报道了一种Co-N掺杂介观/微孔碳催化剂（Co/N/MPC-act）的简便合成路线，该路线通过间苯二酚基树脂、三嵌段共聚物和含Co离子液体的自组装，然后进行CO2活化。所得催化剂在碱性介质中表现出优异的氧还原活性。它产生 0.960 V（相对于 RHE）的起始电位和 5.0 mA/cm2 的极限电流密度，与商用 Pt/C 催化剂相当。这种高活性是由相互连接的介观/微孔结构和高度分散的CoNx物种与金属Co的组合所促成的。Co/N/MPC-act催化剂表现出优异的长期运行稳定性和甲醇耐受性，使其成为一种有前途的用于质子交换膜燃料电池的非贵金属基ORR催化剂。
Proton-exchange-membrane fuel cells (PEMFCs) are of considerable interest as a sustainable, renewable, efficient, and eco-friendly electrochemical conversion systems of energy. Sluggish oxygen reduction reaction (ORR) as the cathodic reaction have mainly dragged down the PEMFCs in practical use. The most effective catalyst for ORR today is a Pt-based catalyst, which have a high scarcity value and low durability for methanol. Therefore, major efforts have recently been devoted to exploring transition metal and hetero-atom doped carbon materials in fuel cells for large-scale and commercial applications. Herein, we report a facile synthesis route of Co-N doped meso/microporous carbon catalysts (Co/N/MPC-act) via self-assembly of resorcinol-based resin, triblock co-polymer and Co containing ionic liquid followed by CO2activation. The obtained catalyst exhibited outstanding oxygen reduction activity in an alkaline medium. It yields an onset potential of 0.960 V (vs. RHE) and a limiting current density of 5.0 mA/cm2, which are comparable to that of the commercial Pt/C catalyst. This high activity is contributed by the combination of inter-connected meso/microporous structures and highly dispersed CoNxspecies with metallic Co. The Co/N/MPC-act catalyst exhibited excellent long-term operation stability and methanol tolerance, making it a promising non-precious metal-based ORR catalyst for PEMFCs.