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Simple Route for the Synthesis of Highly Active Bimetallic Nanoparticle Catalysts with Immiscible Ru and Ni Combination by utilizing a TiO2 Support
ChemCatChem ( IF 4.5 ) Pub Date : 2018-07-05 , DOI: 10.1002/cctc.201800329
Shinya Masuda,Kohsuke Mori,Taiki Sano,Kohei Miyawaki,Wei-Hung Chiang,Hiromi Yamashita

TiO2 support was proven to be acted as an efficient platform for the synthesis of RuNi bimetallic alloy, which are essentially immiscible at most of equilibrium composition, by simple impregnation followed by H2 reduction at 300 °C. Characterization by means of HAADF‐STEM and EDX analysis confirmed the formation of RuNi bimetallic nanoparticles (NPs) with a mean diameter of 2.3 nm. H2‐TPR and in situ XAFS measurements suggested the intraparticle hydrogen spillover mechanism on the surface of TiO2, which originated from the improved reducibility of the Ni species and retarded reducibility of the Ru species in comparison with those for the monometallic samples. RuNi/TiO2 catalyst exhibits remarkably high catalytic activity for the dehydrogenation from ammonia borane (AB, NH3BH3) (TOF=914 min−1) compared with those prepared with other conventional supports. DFT calculation study also suggested the synergistic alloying effect due to the random distribution of Ru−Ni NPs plays a crucial role in the improvement of the adsorption energy of AB, which ultimately resulted in the exceptional catalytic performance.

中文翻译:

利用TiO2载体合成Ru和Ni不混溶的高活性双金属纳米催化剂的简单方法

TiO 2载体被证明是合成RuNi双金属合金的有效平台,RuNi双金属合金通过简单的浸渍,然后在300°C下还原H 2,在大多数平衡组成下基本上是不混溶的。通过HAADF-STEM和EDX分析进行的表征证实了平均直径为2.3 nm的RuNi双金属纳米颗粒(NPs)的形成。H 2 -TPR和原位XAFS测量表明,在TiO 2表面上存在颗粒内氢溢出机制,这是由于与单金属样品相比,Ni物种的还原性提高,Ru物种的还原性降低。RuNi / TiO 2与用其他常规载体制备的催化剂相比,该催化剂显示出从氨硼烷(AB,NH 3 BH 3)脱氢的显着高催化活性(TOF = 914min -1)。DFT计算研究还表明,由于Ru-Ni NPs的随机分布而产生的协同合金化作用在提高AB的吸附能方面起着至关重要的作用,最终导致了优异的催化性能。
更新日期:2018-07-05
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