Introducing dual metal centers in high purity pyrrolic-N for superior oxygen reduction reaction

Hao，Rui1,2; Gu，Shuai1; Hu，Jing1,3; Chen，Jingjing1; Gan，Qingmeng1; Li，Yingzhi1; Wang，Zhiqiang1; Liu，Guiyu1; Yan，Chunliu1; Yuan，Huimin1; Liu，Kaiyu2; Liu，Chen3; Lu，Zhouguang1

2023-06-05

10.1016/j.carbon.2023.118031

Carbon   影响因子和分区

0008-6223

1873-3891

Transition metal- and N-codoped carbon catalysts with low cost are latent substitutes to Pt-based catalysts in oxygen reduction reaction. However, the variety of N species obtained by pyrolysis often makes the determination of the active site controversial. Here, we design catalyst structures with pyrrolic-N anchored dual metal centers, while the presence of pyrrolic-N avoids the complex and variable structure of the active sites. Theory calculations demonstrate that coupling of the Cu–N single-atom sites is favorable to reduce the reaction energy barrier of pyrrolic-N-type Fe–N active site during the reaction process. Subsequently, the high-purity pyrrolic-N-type iron and copper single-atom catalyst is successfully synthesized to verify the hypothesis. The obtained FeCu–N–C catalyst achieves a half-wave potential of 0.913 V, higher than the 0.839 V of Pt/C. This route may provide new insights for regulating catalytic active sites in high purity pyrrolic-N type catalysts.

DFT Dual metal centers Oxygen reduction reaction Pyrrolic-N Single-atom catalyst

SCI ; EI

英语

第一 ; 通讯

Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[JCYJ20200109141640095] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Natural Science Foundation of Guangdong Province[2022A1515011438] ; National Natural Science Foundation of China["U22A20439","22272204"] ; Jiangsu Key Laboratory of Electro-chemical Energy Storage Technologies[EEST2021-1] ; China Post-doctoral Science Foundation[2022M722168] ; Stable Support Plan Program of Shenzhen Natural Science Fund[20200925154236004]

Chemistry ; Materials Science

Chemistry, Physical ; Materials Science, Multidisciplinary

WOS:000983297300001

PERGAMON-ELSEVIER SCIENCE LTD

20231613902232

Atoms ; Catalyst activity ; Design for testability ; Oxygen ; Transition metals

Metallurgy and Metallography:531 ; Ore Treatment:533.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

CHEMISTRY

2-s2.0-85152597025

Scopus

1.Department of Materials Science and Engineering,Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials,Southern University of Science and Technology,Shenzhen,518055,China
2.Hunan Provincial Key Laboratory of Chemical Power Sources,College of Chemistry and Chemical Engineering,Central South University,Changsha,410083,China
3.Guangdong Research Center for Interfacial Engineering of Functional Materials,College of Materials Science and Engineering,Shenzhen University,Shenzhen,518060,China

Hao，Rui,Gu，Shuai,Hu，Jing,et al. Introducing dual metal centers in high purity pyrrolic-N for superior oxygen reduction reaction[J]. Carbon,2023,209.

Hao，Rui.,Gu，Shuai.,Hu，Jing.,Chen，Jingjing.,Gan，Qingmeng.,...&Lu，Zhouguang.(2023).Introducing dual metal centers in high purity pyrrolic-N for superior oxygen reduction reaction.Carbon,209.

Hao，Rui,et al."Introducing dual metal centers in high purity pyrrolic-N for superior oxygen reduction reaction".Carbon 209(2023).