Yan Yan, Yu Rui, Liu Mingkai, Qu Zehua, Yang Jifeng, He Siyuan, Li Hongliang, Zeng Jie
Anhui University of Technology, Ma'anshan, Anhui, 243002, P. R. China.
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, 200433, China.
Nat Commun. 2025 Jan 2;16(1):334. doi: 10.1038/s41467-024-55630-y.
A potential non-precious metal catalyst for oxygen reduction reaction should contain metal-N moieties. However, most of the current strategies to regulate the distances between neighboring metal sites are not pre-designed but depend on the probability by tuning the metal loading or the support. Herein, we report a general method for the synthesis of neighboring metal-N moieties (metal = Fe, Cu, Co, Ni, Zn, and Mn) via an interfacial-fixing strategy. Specifically, polydopamine is used to coat nanotemplates made of metal oxides, followed by pyrolysis to form a metal-oxide skeleton coated by rich nitrogen-doped carbon shells. After chemically etching the skeleton, only interfacial metal atoms strongly bonded with the support via nitrogen atoms are retained. The high purity (>95%) of dual Fe sites was confirmed by both the direct visualization of local regions and the indirect evidence of the averaged information. When these neighboring metal-N moieties are applied for oxygen reduction reaction, Fe-N moieties exhibit the superior activity, even outperforming commercial Pt/C in the aspects of the half-wave potential, methanol tolerance, carbon monoxide tolerance, and robustness.
一种潜在的用于氧还原反应的非贵金属催化剂应包含金属 - N部分。然而，目前大多数调节相邻金属位点之间距离的策略并非预先设计的，而是依赖于通过调整金属负载量或载体来实现的概率。在此，我们报道了一种通过界面固定策略合成相邻金属 - N部分（金属 = 铁、铜、钴、镍、锌和锰）的通用方法。具体而言，聚多巴胺用于包覆由金属氧化物制成的纳米模板，随后进行热解以形成由富含氮掺杂碳壳包覆的金属氧化物骨架。化学蚀刻骨架后，仅保留通过氮原子与载体强烈结合的界面金属原子。通过局部区域的直接可视化和平均信息的间接证据证实了双铁位点的高纯度（>95%）。当这些相邻金属 - N部分应用于氧还原反应时，铁 - N部分表现出优异的活性，甚至在半波电位、甲醇耐受性、一氧化碳耐受性和稳定性方面优于商业铂碳。
