Decarolis Donato, Lezcano-Gonzalez Ines, Gianolio Diego, Beale Andrew M
1Chemistry Department, University College London, 20 Gordon Street, London, WC1H 0AJ UK.
2Rutherford Appleton Laboratory, Research Complex at Harwell, Harwell Science and Innovation Campus, Harwell Didcot, Oxon, OX11 0FA UK.
Top Catal. 2018;61(3):162-174. doi: 10.1007/s11244-018-0887-4. Epub 2018 Jan 19.
Pd nanoparticles supported on SiO, SiN and AlO were studied to examine the effect of particle size and support type on the hydrogenation of 1,3-butadiene. Pd nanoparticles were produced using a reverse micelle method resulting in particles with a remarkably small particle size distribution (σ < < 1 nm). The support type and particle size were observed to affect both catalytic activity and product selectivity. All catalysts showed a decrease of their activity with time on stream, paired with an increase in selectivity to butenes (1-butene and /-2-butene) from a product stream initially dominated by -butane. In situ XAFS demonstrated a correlation between the formation of palladium hydride and -butane production in the early stages (~ 1 h) of reaction. The extent of palladium hydride formation, as well as its depletion with time on stream, was dependent on both particle size and support type. Metallic Pd was identified as the species selective towards the production of butenes.
研究了负载在SiO、SiN和AlO上的钯纳米颗粒，以考察粒径和载体类型对1,3 - 丁二烯氢化反应的影响。采用反胶束法制备钯纳米颗粒，得到粒径分布非常窄（σ << 1 nm）的颗粒。观察到载体类型和粒径对催化活性和产物选择性均有影响。所有催化剂的活性均随反应时间延长而降低，同时产物选择性从最初以丁烷为主的产物流中对丁烯（1 - 丁烯和/ - 2 - 丁烯）的选择性增加。原位XAFS表明，在反应初期（约1小时），氢化钯的形成与丁烷生成之间存在相关性。氢化钯的形成程度及其随反应时间的消耗，均取决于粒径和载体类型。金属钯被确定为对丁烯生成具有选择性的物种。
