水体系中钌催化不饱和有机物加氢反应研究
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摘要
水不仅安全、便宜、环境友好,而且在很多化学化工过程中有着不可或缺的作用。上世纪80年代以来,科学家们不断发现水不仅能提高某些反应的活性,还能具有特定的选择性;而催化剂易于分离则一直是水/有机反应体系的优势所在。本论文考察了水存在条件下的苯选择加氢反应,水溶液中链状钌纳米阵列的制备及其在含水体系中不饱和有机物快速全加氢反应中的应用。
论文采用负载型纳米钌基催化剂和负载型非晶态合金钌硼催化剂对水存在条件下苯选择加氢合成环己烯反应进行了较为系统的研究。研究发现,负载型非晶态合金催化剂H-204在苯选择加氢反应中,显示出很好的催化性能。在苯转化率为40%时,环己烯的选择性达到77%,此时的TOF值为315h~(-1)。
论文采用聚合物参与的水溶液法,制备出直径1-3nm,长约280nm的链状钌纳米阵列。通过调整PVP的平均分子量、PVP单体与钌的摩尔比和氢气的分压,可以得到各种形态的链状钌纳米阵列。该纳米阵列,在353K,1MPa氢压下,对从10mg/l到10,000mg/l相当宽的浓度范围内的苯酚水溶液的催化加氢反应都显示出很高的活性。
论文采用含有链状钌纳米阵列的PVP-Ru两亲性微反应器体系,353K,4MPa氢压下,实现了水/有机体系不饱和化合物的快速全加氢反应。该体系表现出优异的催化活性和底物普适性。其中,苯加氢反应的TOF值达到45,000 h~(-1)。据我们所知,这个值是目前文献报道中最高的。其它苯的衍生物、不饱和羰基化合物以及在水中溶解度极低的长链烯烃加氢反应的起始TOF值也都超过1,000 h~(-1)。
Water is not only safe,cheap and environmental friendly, but also play important roles in chemical industry. Since 1980s, scientists found that water could enhance some reactions’rates, elicit new selectivities, and water-soluble catalysts could be reused after easy separation from the water-insoluble products in aqueous/organic system. This paper studied the selective hydrogenation of benzene to cyclohexene, preparation of chain-like Ru nanoparticle arrays and its application in fast hydrogenation of unsaturated compounds in aqueous media. In this paper, supported ruthenium nanoparticle catalysts and supported amorphous Ru-B catalysts were used in selective hydrogenation of benzene to cyclohexene. Supported amorphous catalysts H-204 showed high selectivity to cyclohexene. When benzene conversion was 40%, the selectivity of cyclohexene reached 77% and the TOF value was 315 h~(-1).
Chain-like Ru nanoparticle arrays, 1-3 nm in diameter and ~280 nm in length, had been successfully synthesized through polymer-mediated aqueous-solution method. The morphology of these Ru nanoparticle arrays could be varied from long chain-like arrays to cross-linked arrays by adjusting the reaction conditions including the average molecular weight of PVP, the mole ratio of repeat unit of PVP to Ru and concentration of hydrogen in solution. The obtained chain-like Ru nanoparticle arrays showed high activity in catalytic hydrogenation of phenol with broad concentration ranging from 10 mg/l to 10,000 mg/l at 353 K, under 1 MPa
论文采用负载型纳米钌基催化剂和负载型非晶态合金钌硼催化剂对水存在条件下苯选择加氢合成环己烯反应进行了较为系统的研究。研究发现,负载型非晶态合金催化剂H-204在苯选择加氢反应中,显示出很好的催化性能。在苯转化率为40%时,环己烯的选择性达到77%,此时的TOF值为315h~(-1)。
论文采用聚合物参与的水溶液法,制备出直径1-3nm,长约280nm的链状钌纳米阵列。通过调整PVP的平均分子量、PVP单体与钌的摩尔比和氢气的分压,可以得到各种形态的链状钌纳米阵列。该纳米阵列,在353K,1MPa氢压下,对从10mg/l到10,000mg/l相当宽的浓度范围内的苯酚水溶液的催化加氢反应都显示出很高的活性。
论文采用含有链状钌纳米阵列的PVP-Ru两亲性微反应器体系,353K,4MPa氢压下,实现了水/有机体系不饱和化合物的快速全加氢反应。该体系表现出优异的催化活性和底物普适性。其中,苯加氢反应的TOF值达到45,000 h~(-1)。据我们所知,这个值是目前文献报道中最高的。其它苯的衍生物、不饱和羰基化合物以及在水中溶解度极低的长链烯烃加氢反应的起始TOF值也都超过1,000 h~(-1)。
Water is not only safe,cheap and environmental friendly, but also play important roles in chemical industry. Since 1980s, scientists found that water could enhance some reactions’rates, elicit new selectivities, and water-soluble catalysts could be reused after easy separation from the water-insoluble products in aqueous/organic system. This paper studied the selective hydrogenation of benzene to cyclohexene, preparation of chain-like Ru nanoparticle arrays and its application in fast hydrogenation of unsaturated compounds in aqueous media. In this paper, supported ruthenium nanoparticle catalysts and supported amorphous Ru-B catalysts were used in selective hydrogenation of benzene to cyclohexene. Supported amorphous catalysts H-204 showed high selectivity to cyclohexene. When benzene conversion was 40%, the selectivity of cyclohexene reached 77% and the TOF value was 315 h~(-1).
Chain-like Ru nanoparticle arrays, 1-3 nm in diameter and ~280 nm in length, had been successfully synthesized through polymer-mediated aqueous-solution method. The morphology of these Ru nanoparticle arrays could be varied from long chain-like arrays to cross-linked arrays by adjusting the reaction conditions including the average molecular weight of PVP, the mole ratio of repeat unit of PVP to Ru and concentration of hydrogen in solution. The obtained chain-like Ru nanoparticle arrays showed high activity in catalytic hydrogenation of phenol with broad concentration ranging from 10 mg/l to 10,000 mg/l at 353 K, under 1 MPa
引文
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