乙炔
催化作用
贵金属
反应性(心理学)
材料科学
选择性
碳纤维
热解
密度泛函理论
扩展X射线吸收精细结构
金属有机骨架
吸收(声学)
光化学
无机化学
吸收光谱法
物理化学
化学
有机化学
计算化学
物理
替代医学
医学
病理
量子力学
复合数
复合材料
吸附
作者
Shengjie Wei,Xingwu Liu,Chao Wang,Xingchen Liu,Qinghua Zhang,Zhi Li,Qinghua Zhang,Zhi Li
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-07-18
卷期号:17 (15): 14831-14839
被引量:31
标识
DOI:10.1021/acsnano.3c03078
摘要
Rationally designing efficient catalysts for semi-hydrogenation of acetylene is significant but challenging. Herein, Pd isolated single-atom sites (ISAS) on a covalent-organic-framework (COF)-derived nanosphere (Pd-ISAS/CN) are synthesized by a COF-absorption-pyrolysis strategy. This synthetic strategy is also applicable for Pt and Ru ISAS catalysts, demonstrating that it is a general method to synthesize noble-metal ISAS on COF-derived carbon materials. Pd-ISAS/CN exhibits outstanding reactivity and high selectivity for semi-hydrogenation of acetylene, with 92% conversion of acetylene, 80% selectivity toward ethylene at 100 °C, and corresponding activity is as high as 712 molacetylene molmetal-1 h-1. Extended X-ray absorption fine structure (EXAFS) measurement and density functional theory (DFT) calculation reveal the Pd-N1C3 sites from Pd-ISAS/CN efficiently boost the reactivity for semi-hydrogenation of acetylene. This work will bring inspiration to rationally design noble-metal-based ISAS catalysts derived from COF materials and boost catalytic performance by optimizing the coordination environment of catalytic sites.
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