Porphyrin polymer-derived single-atom Fe assisted by Fe2O3 with oxygen vacancy for efficient oxygen reduction reaction

被引:18
|
作者
Ren, Jianwei [1 ]
Yan, Wei [2 ]
Liu, Xue [2 ]
Wang, Fuling [1 ]
Xing, Qianli [1 ]
Xiao, Zuoxu [1 ]
Liu, Heyuan [1 ]
Chen, Yanli [2 ]
Li, Xiyou [2 ]
机构
[1] China Univ Petr East China, Coll Chem & Chem Engn, Qingdao 266580, Peoples R China
[2] China Univ Petr East China, Sch Mat Sci & Engn, Qingdao 266580, Peoples R China
基金
中国国家自然科学基金;
关键词
Oxygen reduction reaction; Fe2O3; Oxygen vacancy; Porphyrin conjugated mesoporous polymer; Zinc-air battery; POROUS CARBON; ELECTROCATALYST; CATALYSTS; ALKALINE; IRON; FRAMEWORKS; NITROGEN; SITES; EDGE;
D O I
10.1016/j.apsusc.2022.153301
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Single-atom catalysts (SACs) have been deemed as one of the most prospective substitutes for high-efficiency oxygen reduction reaction (ORR) catalysts due to its theoretical maximum atomic utilization. However, the convenient preparation and the further improvement in activity of SACs are laborious. Herein, the N-doped porous carbon (NC) material with in site produced Fe-N-4 single-atom catalytic sites (FeSA) accompanied by Fe2O3 species with abundant oxygen vacancies (Ov-Fe2O3) as co-catalytic sites (Ov-Fe2O3@FeSA@NC) is successfully obtained by using a well-designed porphyrin conjugated mesoporous polymer (CMP) consisting of iron porphyrin and metal free porphyrin units as a precursor, and followed by pyrolysis. A series of controllable experiments reveal that FeSA assisted by Ov-rich Fe2O3 render Ov-Fe2O3@FeSA@NC outstanding ORR activity in the alkaline medium with the onset and half-wave potentials (E-onset and E-1/2) of 0.987 V and 0.901 V vs RHE, which significantly outperformed the electrochemical activity of FeSA@NC (E-onset = 0.962 V, E1/2 = 0.850 V) and Ov-Fe2O3@NC (E-onset = 0.913 V, E1/2 = 0.821 V) with individual FeSA and Ov-Fe2O3 active sites, respectively. This work innovatively demonstrates the importance of oxygen vacancy-assisted single-atom catalysts for oxygen reduction catalysis, and also provides guidance for the design of high-performance SACs.
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页数:8
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