Tuning the interfaces in the ruthenium-nickel/carbon nanocatalysts for enhancing catalytic hydrogenation performance

Tuning the interfaces in the ruthenium-nickel/carbon nanocatalysts for enhancing catalytic hydrogenation performance
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调整钌镍/碳纳米催化剂的界面以提高催化加氢性能

DOI:
10.1016/j.jcat.2019.07.041
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发表时间:
2019-09
影响因子:
7.3
通讯作者:
Bing Hui Chen
Bing Hui Chen
中科院分区:
化学1区
文献类型:
--
作者:
Lihua Zhu;Huan Zhang;Nan Ma;Changlin Yu;Nengwen Ding;Jeng-Lung Chen;Chih-Wen Pao;Jyh-Fu Lee;Qiang Xiao;Bing Hui Chen

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在保持Ru/Ni原子比(51/49)不变的条件下,以水合肼为还原剂,采用电偶置换反应方法,在常温下合成了不同Ru和Ni负载量的Ru-Ni/C双金属纳米颗粒。将Ru-Ni-NiO(1.250 或0.630 wt%Ru)和RuO2-NiO(Ru 0.160 wt%Ru)在氮气中于380 °C下退火3 h,形成了不同的Ru-Ni界面,并用粉末X射线衍射仪、透射电子显微镜、高分辨电子显微镜、同步辐射X射线吸收光谱和氢气中原位X射线吸收光谱对其结构进行了表征。结果表明,Ru-Ni-NiO界面上的大部分Ru原子和少量Ni原子被还原,导致氢溢出,从而导致Ru、Ni和NiO活性中心的协同效应。然而,在RuO2-NiO界面上没有观察到这样的协同作用。由于存在特殊的Ru-Ni-NiO界面,Ru-Ni/C纳米催化剂在苯加氢反应中的催化性能显著提高。
The ruthenium-nickel bimetallic nanoparticles supported on carbon black (Ru-Ni/C) with various Ru and Ni loadings, while keeping a constant Ru/Ni atomic ratio (51/49), were synthesized at ambient temperature by liquid reduction with hydrazine hydrate as reducing agent and galvanic replacement reaction approaches. Different Ru-Ni interfaces (Ru-Ni-NiO with 1.250 wt% or 0.630 wt% Ru, and RuO2-NiO with 0.160 wt% Ru) were formed after being annealed in N2at 380 °C for 3 h. Several techniques, including powder X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution TEM (HRTEM) and synchrotron radiation X-ray absorption spectroscopy (XAS) and in-situ XAS (in hydrogen) have been employed for structural characterization. It was found that most Ru atoms and a small amount of Ni atoms at the Ru-Ni-NiO interface were reduced, leading to the occurrence of hydrogen spillover and hence synergy effect of Ru, Ni and NiO active sites. However, such a synergy was not observed at the RuO2-NiO interface. The catalytic properties of the Ru-Ni/C nanocatalysts in the hydrogenation of benzene reaction were significantly improved due to the presence of particular Ru-Ni-NiO interface.
通过原位表面增强拉曼光谱揭示界面性质对催化行为的作用
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