化工进展

• 工业催化 • 上一篇    下一篇

合成气制C2含氧化合物Rh基催化剂中的载体效应

陈维苗1,丁云杰1,2,薛飞1,3,宋宪根1,朱何俊1,吕元1   

  1. 1中国科学院大连化学物理研究所洁净能源国家实验室(筹),辽宁 大连 116023;2中国科学院大连化学物理研究所催化重点国家实验室,辽宁 大连 116023;3中国科学院大学,北京100039
  • 出版日期:2014-07-05 发布日期:2014-07-25

Support effect of Rh-based catalyst for CO hydrogenation to C2-oxygenates

CHEN Weimiao1,DING Yunjie1,2,XUE Fei1,3,SONG Xiangen1,ZHU Hejun1,Lü Yuan1   

  1. 1Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Science,Dalian 116023,Liaoning,China;2 State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics, Chinese Academy of Science,Dalian 116023,Liaoning,China;3University of the Chinese Academy of Science,Beijing 100039,China
  • Online:2014-07-05 Published:2014-07-25

摘要: 负载型Rh基催化剂是实现由煤或生物质经合成气制乙醇等C2含氧化合物过程的最高效催化剂之一,其中载体的选择至关重要。本文综述了硅胶、Al2O3、TiO2、多孔炭材料、分子筛和复合氧化物等载体负载的Rh基催化剂性能及其研究进展,阐明了载体中的杂质、孔道结构、酸碱性、表面基团性质和可还原性等性质如何影响催化剂活性组分的物化性质乃至催化性能。结果表明,载体与活性组分(助剂)间的相互作用机制和程度是理解载体效应的关键。因此,应设计和制备出具有适宜孔结构、表面活性和可还原性适中、略偏碱性的催化剂载体,同时细致优化催化剂制备和活化过程,以达到适宜的金属-载体相互作用,确保产生更多的催化活性位,从而最大限度地提高Rh的催化效率,推动该过程的工业化进程。

关键词: 一氧化碳, 加氢, 铑, 催化剂, 乙醇, C2含氧化合物, 载体效应, 金属-载体相互作用, 硅胶

Abstract: Supported Rh-based catalysts are one of the most efficient catalysts for CO hydrogen to C2-oxygenates,such as ethanol from coal or biomass via syngas,however,the selection of support is vitally important for the design and preparation of the catalyst. Herein,the catalytic performances and the research progresses of silica,Al2O3,TiO2,porous carbon materials,zeolites,and mixed oxides supported Rh-based catalysts were reviewed. The effects of support properties,such as the impurities,pore structures,acid-base properties,the reactivity of surface groups,and reducibility,on the chemical-physical properties and thus catalytic performance of Rh-based catalysts were compared and summarized. The results showed that the key point to understand the support effect was to investigate the interactions between metal (promoters) and support. Accordingly,novel support with proper pore structures,weakly basic,moderate surface reactivity and reducibility should be designed and synthesized,which could modify the interaction between support and Rh combing with the optimization of preparation and activation conditions. This ensures more active sites for syngas conversion and thus makes the maximum use of Rh,pushing the commercialization of this process.

Key words: carbon oxide, hydrogenation, rhodium, catalyst, ethanol, C2-oxygenates, support effect, metal-support interaction, silica