Lin Yunxiang, Geng Bo, Zheng Ruyun, Chen Wei, Zhao Jiahui, Liu Hengjie, Qi Zeming, Yu Zhipeng, Xu Kun, Liu Xue, Yang Li, Shan Lei, Song Li
Institutes of Physical Science and Information Technology, Leibniz International Joint Research Center of Materials Sciences of Anhui Province, Anhui University, Hefei, 230601, China.
Center of Free Electron Laser & High Magnetic Field, School of Materials Science and Engineering, Anhui University, Hefei, 230601, China.
Nat Commun. 2025 Jan 2;16(1):286. doi: 10.1038/s41467-024-55615-x.
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 NiFeN lattice are synthesized and studied as a typical case over alkaline methanol electrooxidation. The NiFeN with buried Ru atoms in subsurface lattice (NiFeN-Ru) exhibits high selectivity and Faradaic efficiency of methanol to formate conversion. Meanwhile, operando spectroscopies reveal that the NiFeN-Ru exhibits an optimized adsorption of reactants along with an inhibited surface structural reconstruction. Additional theoretical simulations demonstrate that the NiFeN-Ru 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.
对于单原子催化剂而言，精确制备和调控具有所需性能的稳定催化剂仍然具有挑战性。在此，合成并研究了在NiFeN晶格中具有不同配位环境的Ru单原子，作为碱性甲醇电氧化的典型案例。在次表面晶格中埋入Ru原子的NiFeN（NiFeN-Ru）对甲醇转化为甲酸盐表现出高选择性和法拉第效率。同时，原位光谱表明，NiFeN-Ru对反应物具有优化的吸附作用，同时抑制了表面结构重构。额外的理论模拟表明，NiFeN-Ru显示出表面金属原子的局部电子态得到调控，反应物吸附得到优化，且电位决定步骤的能垒降低。这项工作不仅报道了一种在碱性条件下将甲醇转化为甲酸盐的高效催化剂，还为合理设计具有更多可及表面活性位点的单原子催化剂提供了思路。
