相邻的原子铂位点使单原子铁具有高氧还原反应性能。
An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance.
作者信息
Han Ali, Wang Xijun, Tang Kun, Zhang Zedong, Ye Chenliang, Kong Kejian, Hu Haibo, Zheng Lirong, Jiang Peng, Zhao Changxin, Zhang Qiang, Wang Dingsheng, Li Yadong
机构信息
Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, China.
出版信息
Angew Chem Int Ed Engl. 2021 Aug 23;60(35):19262-19271. doi: 10.1002/anie.202105186. Epub 2021 Jul 21.
The modulation effect has been widely investigated to tune the electronic state of single-atomic M-N-C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in-depth study of modulation effect is rarely reported for the isolated dual-atomic metal sites. Now, the catalytic activities of Fe-N moiety can be enhanced by the adjacent Pt-N moiety through the modulation effect, in which the Pt-N acts as the modulator to tune the 3d electronic orbitals of Fe-N active site and optimize ORR activity. Inspired by this principle, we design and synthesize the electrocatalyst that comprises isolated Fe-N /Pt-N moieties dispersed in the nitrogen-doped carbon matrix (Fe-N /Pt-N @NC) and exhibits a half-wave potential of 0.93 V vs. RHE and negligible activity degradation (ΔE =8 mV) after 10000 cycles in 0.1 M KOH. We also demonstrate that the modulation effect is not effective for optimizing the ORR performances of Co-N /Pt-N and Mn-N /Pt-N systems.
为了调节单原子M-N-C催化剂的电子态以增强氧还原反应（ORR）的活性，人们对调制效应进行了广泛研究。然而，对于孤立的双原子金属位点，关于调制效应的深入研究却鲜有报道。现在，通过调制效应，相邻的Pt-N部分可以增强Fe-N部分的催化活性，其中Pt-N作为调节剂来调节Fe-N活性位点的3d电子轨道并优化ORR活性。受这一原理的启发，我们设计并合成了一种电催化剂，它由分散在氮掺杂碳基质中的孤立Fe-N/Pt-N部分组成（Fe-N/Pt-N@NC），在0.1 M KOH中，其相对于可逆氢电极（RHE）的半波电位为0.93 V，并且在10000次循环后活性降解可忽略不计（ΔE = 8 mV）。我们还证明，调制效应对于优化Co-N/Pt-N和Mn-N/Pt-N体系的ORR性能无效。
Zotero 插件