Tuning the coordination environment in single-atom catalysts to achieve highly efficient oxygen reduction reactions
學年 108
學期 1
出版（發表）日期 2019-12-05
作品名稱 Tuning the coordination environment in single-atom catalysts to achieve highly efficient oxygen reduction reactions
作品名稱（其他語言）
著者 J. Zhang, Y. Zhao, C. Chen, Y. C. Huang, C. L. Dong, C. J. Chen, R. S. Liu, C. Wang, K. Yan, Y. Li, G. Wang
單位
出版者
著錄名稱、卷期、頁數 J. Am. Chem. Soc. 141(51), p.20118-20126
摘要 Designing atomically dispersed metal catalysts for oxygen reduction reaction (ORR) is a promising approach to achieve efficient energy conversion. Herein, we develop a template-assisted method to synthesize a series of single metal atoms anchored on porous N,S-codoped carbon (NSC) matrix as highly efficient ORR catalysts to investigate the correlation between the structure and their catalytic performance. The structure analysis indicates that an identical synthesis method results in distinguished structural differences between Fe-centered single-atom catalyst (Fe-SAs/NSC) and Co-centered/Ni-centered single-atom catalysts (Co-SAs/NSC and Ni-SAs/NSC) because of the different trends of each metal ion in forming a complex with the N,S-containing precursor during the initial synthesis process. The Fe-SAs/NSC mainly consists of a well-dispersed FeN4S2 center site where S atoms form bonds with the N atoms. The S atoms in Co-SAs/NSC and Ni-SAs/NSC, on the other hand, form metal–S bonds, resulting in CoN3S1 and NiN3S1 center sites. Density functional theory (DFT) reveals that the FeN4S2 center site is more active than the CoN3S1 and NiN3S1 sites, due to the higher charge density, lower energy barriers of the intermediates, and products involved. The experimental results indicate that all three single-atom catalysts could contribute high ORR electrochemical performances, while Fe-SAs/NSC exhibits the highest of all, which is even better than commercial Pt/C. Furthermore, Fe-SAs/NSC also displays high methanol tolerance as compared to commercial Pt/C and high stability up to 5000 cycles. This work provides insights into the rational design of the definitive structure of single-atom catalysts with tunable electrocatalytic activities for efficient energy conversion.
關鍵字
語言 en
ISSN 1520-5126
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 否
國別 USA
公開徵稿
出版型式 ,電子版
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