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Alcohol amination over titania-supported ruthenium nanoparticles
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-05-27 , DOI: 10.1039/d0cy00709a Feng Niu 1, 2, 3, 4, 5 , Shaohua Xie 1, 2, 3, 4, 5 , Zhen Yan 6, 7, 8, 9 , Bright T. Kusema 6, 7, 8, 9 , Vitaly V. Ordomsky 1, 2, 3, 4, 5 , Andrei Y. Khodakov 1, 2, 3, 4, 5
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-05-27 , DOI: 10.1039/d0cy00709a Feng Niu 1, 2, 3, 4, 5 , Shaohua Xie 1, 2, 3, 4, 5 , Zhen Yan 6, 7, 8, 9 , Bright T. Kusema 6, 7, 8, 9 , Vitaly V. Ordomsky 1, 2, 3, 4, 5 , Andrei Y. Khodakov 1, 2, 3, 4, 5
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Metal nanoparticles for heterogeneous catalytic reactions are often supported on porous materials. The catalytic performance of supported catalysts usually depends on the size of the metal nanoparticles and catalytic supports. Selective synthesis of valuable primary amines is an important target in the modern industry. In this work, the catalytic performance of TiO2 supported Ru nanoparticles with sizes from 1.4 to 9.9 nm was investigated in both direct gas-phase amination of 1-butanol and liquid-phase amination of 1-octanol into primary amines in the presence of ammonia. Our results suggest that ruthenium nanoparticle size is one of the most important parameters, which affects the catalytic performance of titania supported catalysts in the amination reactions. The selectivity to primary amines is much higher over smaller supported Ru nanoparticles than over larger ones, especially in the liquid-phase amination of 1-octanol. The 95% selectivity to octylamine is obtained over small supported Ru nanoparticles with a diameter of 1.4 nm even at 95% conversion, whereas for larger Ru nanoparticles, the octylamine selectivity drops as the 1-octanol conversion approached 80–90%. The drop of the selectivity to octylamine at higher conversion is due to the increase in the intrinsic rate of octylamine coupling over larger ruthenium nanoparticles. The support can also contribute to some extent to the rate of primary amine self-coupling, while its effect on the overall catalytic performance is not significant for the titania-supported catalysts.
中文翻译：
二氧化钛负载的钌纳米粒子上的醇胺化
用于多相催化反应的金属纳米粒子通常负载在多孔材料上。负载型催化剂的催化性能通常取决于金属纳米颗粒和催化载体的尺寸。有价值的伯胺的选择性合成是现代工业中的重要目标。在这项工作中，TiO 2的催化性能在1-丁醇的直接气相胺化和在氨存在下将1-辛醇液相胺化成伯胺的过程中，研究了尺寸为1.4至9.9 nm的负载Ru纳米颗粒。我们的结果表明，钌纳米颗粒尺寸是最重要的参数之一，它影响了二氧化钛负载的催化剂在胺化反应中的催化性能。在较小的负载型Ru纳米粒子上，对伯胺的选择性要比较大的Ru纳米粒子高，特别是在1-辛醇的液相胺化中。即使在95％的转化率下，对于直径为1.4 nm的小负载Ru纳米颗粒，辛基胺的选择性也达到95％，而对于较大的Ru纳米颗粒，随着1-辛醇转化率接近80-90％，辛胺的选择性下降。在较高转化率下对辛胺的选择性下降是由于与较大的钌纳米颗粒相比，辛胺偶联的固有速率增加。载体还可以在一定程度上促进伯胺的自偶联速率，而对于二氧化钛负载的催化剂，其对总体催化性能的影响并不明显。
更新日期：2020-07-06
中文翻译：
二氧化钛负载的钌纳米粒子上的醇胺化
用于多相催化反应的金属纳米粒子通常负载在多孔材料上。负载型催化剂的催化性能通常取决于金属纳米颗粒和催化载体的尺寸。有价值的伯胺的选择性合成是现代工业中的重要目标。在这项工作中，TiO 2的催化性能在1-丁醇的直接气相胺化和在氨存在下将1-辛醇液相胺化成伯胺的过程中，研究了尺寸为1.4至9.9 nm的负载Ru纳米颗粒。我们的结果表明，钌纳米颗粒尺寸是最重要的参数之一，它影响了二氧化钛负载的催化剂在胺化反应中的催化性能。在较小的负载型Ru纳米粒子上，对伯胺的选择性要比较大的Ru纳米粒子高，特别是在1-辛醇的液相胺化中。即使在95％的转化率下，对于直径为1.4 nm的小负载Ru纳米颗粒，辛基胺的选择性也达到95％，而对于较大的Ru纳米颗粒，随着1-辛醇转化率接近80-90％，辛胺的选择性下降。在较高转化率下对辛胺的选择性下降是由于与较大的钌纳米颗粒相比，辛胺偶联的固有速率增加。载体还可以在一定程度上促进伯胺的自偶联速率，而对于二氧化钛负载的催化剂，其对总体催化性能的影响并不明显。
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