Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction
Tingyi Zhou,
Yi Guan,
Changjie He,
Lei Zhang,
Xueliang Sun,
Zhongxin Song,
Qianling Zhang,
Chuanxin He,
Xiantao Jiang,
Zhaoyan Luo,
Wei Xing,
Xiangzhong Ren
Affiliations
Tingyi Zhou
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Yi Guan
Department of Mechanical and Materials Engineering University of Western Ontario London Ontario Canada
Changjie He
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Lei Zhang
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Xueliang Sun
Department of Mechanical and Materials Engineering University of Western Ontario London Ontario Canada
Zhongxin Song
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Qianling Zhang
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Chuanxin He
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Xiantao Jiang
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Zhaoyan Luo
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Wei Xing
State Key Laboratory of Electroanalytical Chemistry, Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied Chemistry, Chinese Academy of Sciences Jilin Changchun China
Xiangzhong Ren
College of Chemistry and Environmental Engineering Shenzhen University Shenzhen Guangdong China
Abstract The high‐temperature pyrolysis process for preparing M–N–C single‐atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms (SAs), atomic clusters to nanoparticles. Therefore, understanding the interactions among these components, especially the synergistic effects between single atomic sites and cluster sites, is crucial for improving the oxygen reduction reaction (ORR) activity of M–N–C catalysts. Accordingly, herein, we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation strategy. We found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron‐withdrawing –OH ligands and decreasing the d‐band center of the Fe center. The as‐developed catalyst exhibits encouraging ORR activity with half‐wave potentials (E1/2) of 0.831 and 0.905 V in acidic and alkaline media, respectively. Moreover, the catalyst also represents excellent durability exceeding that of Fe–N–C SA catalyst. The practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metal–air battery device. Our work exhibits the great potential of synergistic effects between multiphase metal species for improvements of single‐atom site catalysts.
