Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation

Yunxiang Lin; Bo Geng; Ruyun Zheng; Wei Chen; Jiahui Zhao; Hengjie Liu; Zeming Qi; Zhipeng Yu; Kun Xu; Xue Liu; Li Yang; Lei Shan; Li Song

doi:10.1038/s41467-024-55615-x

Optimizing surface active sites via burying single atom into subsurface lattice for boosted methanol electrooxidation

Nat Commun. 2025 Jan 2;16(1):286. doi: 10.1038/s41467-024-55615-x.

Authors

Yunxiang Lin^{1

2}, Bo Geng^{1

2}, Ruyun Zheng¹, Wei Chen², Jiahui Zhao¹, Hengjie Liu³, Zeming Qi³, Zhipeng Yu¹, Kun Xu⁴, Xue Liu², Li Yang^{5

6}, Lei Shan^{7

8

9}, Li Song^{10

11}

Affiliations

¹ Institutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui University, Hefei, 230601, China.
² Center of Free Electron Laser & High Magnetic Field, School of Materials Science and Engineering, Anhui University, Hefei, 230601, China.
³ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China.
⁴ School of Chemistry and Chemical Engineering, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, Anhui, 230601, China.
⁵ Institutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui University, Hefei, 230601, China. [email protected].
⁶ School of Chemistry and Chemical Engineering, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, Anhui, 230601, China. [email protected].
⁷ Institutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui University, Hefei, 230601, China. [email protected].
⁸ Center of Free Electron Laser & High Magnetic Field, School of Materials Science and Engineering, Anhui University, Hefei, 230601, China. [email protected].
⁹ Information Meterials and Intelligent Sensing Laboratory of Anhui Province, Anhui University, Hefei, 230601, China. [email protected].
¹⁰ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China. [email protected].
¹¹ Zhejiang Institute of Photonelectronics, Jinhua, Zhejiang, 321004, China. [email protected].

Abstract

The precise fabrication and regulation of the stable catalysts with desired performance still challengeable for single atom catalysts. Here, the Ru single atoms with different coordination environment in Ni₃FeN lattice are synthesized and studied as a typical case over alkaline methanol electrooxidation. The Ni₃FeN with buried Ru atoms in subsurface lattice (Ni₃FeN-Ru_buried) exhibits high selectivity and Faradaic efficiency of methanol to formate conversion. Meanwhile, operando spectroscopies reveal that the Ni₃FeN-Ru_buried exhibits an optimized adsorption of reactants along with an inhibited surface structural reconstruction. Additional theoretical simulations demonstrate that the Ni₃FeN-Ru_buried displays a regulated local electronic states of surface metal atoms with an optimized adsorption of reactants and reduced energy barrier of potential determining step. This work not only reports a high-efficient catalyst for methanol to formate conversion in alkaline condition, but also offers the insight into the rational design of single atom catalysts with more accessible surficial active sites.

Abstract

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