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Low temperature surface oxygen activation in crystalline MnO2 triggered by lattice confined Pd single atoms
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2021-03-24 , DOI: 10.1016/j.jechem.2021.03.012
Xuemei Liao , Yonghui Zhao , Changwen Liu , Xiaopeng Li , Yu Sun , Kenichi Kato , Miho Yamauchi , Zheng Jiang

Tuning the coordination environment is the research axis of single atom catalysts (SACs). SACs are commonly stabilized by various defects from support. Here, we report a lattice confined Pd SAC using MnO2 as support. Compared with the Pd clusters anchored on the surface, the lattice confined Pd single atoms allows spontaneous exaction of surrounding lattice oxygen at room temperature when employed in CO oxidation. The MnO2 supported Pd SAC exhibited a high turnover frequency of 0.203 s−1 at low reaction temperature, which is higher than that of recently reported Pd SACs. Theoretical calculations also confirmed the confined monatomic Pd activate lattice oxygen with an ultralow energy barrier. Our results illustrate that the unique coordination environment of single atom provided by lattice confinement is promising to boost the activity of SACs.



中文翻译:

晶格约束的Pd单原子引发的结晶MnO 2中的低温表面氧活化

调整配位环境是单原子催化剂(SAC)的研究方向。SAC通常通过来自支撑的各种缺陷来稳定。在这里,我们报道了以MnO 2为载体的晶格限制的Pd SAC 。与固定在表面上的Pd团簇相比,当在CO氧化中使用时,晶格受限的Pd单原子可以在室温下自发地包围周围的晶格氧。MnO 2负载的Pd SAC具有0.203 s -1的高周转频率在低反应温度下,该温度高于最近报道的Pd SAC。理论计算也证实了受限的单原子Pd激活了具有超低能垒的晶格氧。我们的结果表明,由晶格限制提供的单个原子的独特配位环境有望提高SAC的活性。

更新日期:2021-04-23
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