| 王鹏,舒新前.CO加氢制备碳二含氧化合物Rh-Nd-V/SiO2催化剂配比的优化[J].分子催化,2014,(2):148-156 |
| CO加氢制备碳二含氧化合物Rh-Nd-V/SiO2催化剂配比的优化 |
| Optimization of Molar Ratio of Rh-Nd-V/SiO2 Catalysts for CO Hydrogenation to C2-Oxygenates |
| 投稿时间：2013-12-27 修订日期：2014-01-22 |
| DOI： |
| 中文关键词: 钕 钒 加氢 碳二含氧化合物 |
| 英文关键词:Neodymium Vanadium Hydrogenation C2-Oxygenates |
| 基金项目:中央高校基本科研业务费专项资金项目 (批准号：2010YH07) |
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| 中文摘要: |
| 采用CO加氢反应、CO吸附和程序升温脱附(CO-TPD)以及程序升温表面反应(TPSR)等方法，考察了助剂Nd和V担载量对Rh-Nd-V/SiO2催化剂上CO加氢合成C2含氧化合物反应性能的影响。研究表明，当助剂Nd和V担载量分别为0.5%和1.0%时，Rh-Nd-V/SiO2 催化剂上C2含氧化合物的选择性和时空产率分别达到59.8%和394.5 g/(kg?h)。CO吸附和TPD实验表明，随着Nd和V担载量的增加，强吸附的CO数量逐渐增加，而弱吸附的CO数量先缓慢增加后又逐渐降低。TPSR实验表明，助剂Nd的添加抑制了CO的解离和加氢能力，而助剂V的添加提高了CO的解离和加氢能力。结合催化反应评价和表征结果，适量助剂Nd和V的添加提高了未解离的CO比例，使得催化剂上可参与插入反应的CO比例增多，催化剂的活性、C2含氧化合物的选择性和时空收率都有所提高。 |
| 英文摘要: |
| Ethanol and other C2-oxygenates are considered to be important chemical raw material, and catalytic synthesis from syngas has attracted more attention to relieve the energy crisis. Rh-based catalysts has been proved the most efficient one on the formation of C2-oxygenates, but the low conversion, poor selectivity and the high cost are insufficient to justify its use, making its commercial available application process limited. The RE and V promoters have showed interesting promotion effects for C2-oxygenates formation, which could boost the activity and selectivity, and both of them together resulted in the excellent performance. More attention were paid to RE elements such as lanthanum, cerium, but little reports about neodymium or neodymium co-promoted rhodium-based catalyst. The influences of Nd and V promoters on the catalytic properties of the Rh-Nd-V/SiO2 catalyst for C2-oxygenate synthesis from CO hydrogenation were investigated. The effects were investigated by pulse adsorption of CO, temperature programmed desorption of CO(CO-TPD) and temperature programmed surface reaction(TPSR). At 563-573K, the Rh efficiency reached the maximum when the Rh loading was 1.0%. The additions of Nd and V enhanced the catalytic performance and selectivity for C2-oxygenates. The selectivity and yield of C2-oxygenates achieved 59.8% and 394.5 g/(kg?h) with the loading amounts of 0.5% Nd and 1.0%V on Rh-Nd-V/SiO2. The CO adsorption and TPD experiments indicated that the amount of strongly adsorbed CO species increased with the additions of Nd and V, while the number of weakly adsorbed CO species increased at first and decreased afterwards. The TPSR results showed the addition of Nd inhibited the dissociation and hydrogenation ability of CO, and addition of Nd was opposite. Combining the above results, the appropriate amounts of Nd and V enhanced the concentration of CO non-dissociated that for inserting, making the catalyst activity, the selectivity and yield of C2 oxygenates a rapid increase. |
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