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Composition-tuned oxidation levels of Pt-Re bimetallic nanoparticles for the etherification of allylic alcohols

机译:用于烯丙基醇醚化的Pt-Re双金属纳米粒子的成分调整氧化水平

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摘要

The catalytic performance of metal nanoparticles is often affected by surface oxidation levels.Instead of post-synthesis oxidation/reduction,we propose an efficient method to modulate the oxidation levels by tuning the composition of bimetallic nanoparticles.Here we report a series of Pt-Re bimetallic nanoparticles synthesized via a facile thermal co-reduction process,with a uniform size of approximately 3 run.The investigation of the growth of the Pt-Re nanoparticles suggests that the Re atoms were enriched on the surface,as confirmed by X-ray photoelectron spectroscopy.Furthermore,X-ray absorption spectroscopy showed that metallic Re was decreased and high-valency ReOx species were increased in particles with higher Re/Pt ratios.In the etherification of allylic alcohols catalyzed by Pt-Re nanoparticles of different compositions under ambient conditions,particles with higher Re/Pt ratios exhibited significantly better performances.The highest mass activity of Pt-Re bimetallic nanoparticles (127 μmol·g-1·s-1) was more than forty times that of the industrial catalyst CH3ReO3 (3 μmol·g-1·s-1).The catalytically active sites were associated with ReOx and could be tuned by adjusting the Pt ratio.
机译:金属纳米颗粒的催化性能通常受表面氧化水平的影响。我们提出了一种通过调节双金属纳米颗粒的组成来调节氧化水平的有效方法,而不是合成后的氧化/还原方法。在此我们报道了一系列的Pt-Re通过便捷的热共还原过程合成的双金属纳米粒子,均匀大小约为3纳米。对Pt-Re纳米粒子生长的研究表明,X射线光电子证实了Re原子在表面富集。 X射线吸收光谱法还表明,具有较高Re / Pt比的颗粒中的金属Re减少而高价ReOx种类增加。在环境条件下,不同组成的Pt-Re纳米颗粒催化的烯丙醇醚化反应,具有较高Re / Pt比的颗粒表现出明显更好的性能。Pt-Re双金属纳米部件的最高质量活性(127μmol·g-1·s-1)的三倍于工业催化剂CH3ReO3(3μmol·g-1·s-1)的四十倍以上。催化活性位点与ReOx相关​​并且可以通过调整Pt比率。

著录项

  • 来源
    《纳米研究(英文版)》 |2018年第11期|5902-5912|共11页
  • 作者单位

    Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering,Peking University, Beijing 100871, China;

    Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering,Peking University, Beijing 100871, China;

    Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering,Peking University, Beijing 100871, China;

    Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China;

    Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering,Peking University, Beijing 100871, China;

    Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications,PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering,Peking University, Beijing 100871, China;

  • 收录信息 中国科学引文数据库(CSCD);中国科技论文与引文数据库(CSTPCD);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-19 04:27:06
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