扩展X射线吸收精细结构
催化作用
化学
铂金
过渡金属
吸收光谱法
密度泛函理论
X射线吸收光谱法
表征(材料科学)
光谱学
金属
吸收(声学)
X射线光谱学
化学物理
纳米技术
结晶学
材料科学
计算化学
有机化学
光学
复合材料
物理
量子力学
作者
Yizhen Chen,Rachita Rana,Tyler Sours,Fernando D. Vila,Shaohong Cao,Thomas Blum,Jiyun Hong,Adam S. Hoffman,Chuo Fang,Zhennan Huang,Chunyan Shang,Chuanhao Wang,Jie Zeng,Miaofang Chi,Coleman X. Kronawitter,Simon R. Bare,Bruce C. Gates,Ambarish Kulkarni
摘要
Atomically dispersed supported metal catalysts offer new properties and the benefits of maximized metal accessibility and utilization. The characterization of these materials, however, remains challenging. Using atomically dispersed platinum supported on crystalline MgO (chosen for its well-defined bonding sites) as a prototypical example, we demonstrate how systematic density functional theory calculations for assessing all the potentially stable platinum sites, combined with automated analysis of extended X-ray absorption fine structure (EXAFS) spectra, leads to unbiased identification of isolated, surface-enveloped platinum cations as the catalytic species for CO oxidation. The catalyst has been characterized by atomic-resolution imaging and EXAFS and high-energy resolution fluorescence detection X-ray absorption near edge spectroscopy. The proposed platinum sites are in agreement with experiment. This theory-guided workflow leads to rigorously determined structural models and provides a more detailed picture of the structure of the catalytically active site than what is currently possible with conventional EXAFS analyses. As this approach is efficient and agnostic to the metal, support, and catalytic reaction, we posit that it will be of broad interest to the materials characterization and catalysis communities.
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