多相催化剂CuY应用于乙炔羰基化合成丙烯酸反应的性能研究
发布时间：2019-06-18 12:44
【摘要】：论文以实现乙炔羰基化合成丙烯酸均相催化剂多相化为目标,制备了一系列固载活性金属组分的双功能催化剂,研究其用于多相反应体系的催化性能。基于本实验室已有的镍基多相催化剂的研究开发经验和基础,本课题主要针对铜基多相催化剂进行研究和开发。课题采用液相离子交换法将铜组份固载到Y分子筛上。同时采用XRD,XPS,ICP-AES,IC,BET,FT-IR,pyridine/CO-IR,NH3-TPD,Raman,TG-DTG 以及SEM多种仪器对催化剂的结构、组分及酸性等多种性质进行表征分析,研究其与催化剂活性之间的相关性,并且对最高效的催化剂进行失活和再生研究,提出积碳生长机理。采用不同铜活性组分前驱体(Cu(NO_3)_2、CuBr_2及CuSO_4)制备的CuY催化剂的表征结果显示,阴离子SO_4~(2-)与催化剂中[CuOCu]~(2+)结合的方式更为有效,可以产生更多、更强的酸性中心,具有更高的催化活性。通过将催化剂前驱体在不同的气氛下(空气、氮气及氢气)焙烧,获得具有丰富铜物种(Cu0、Cu~+、Cu_2O、Cu~(2+)、CuO)分布的催化剂。XPS及pyridine-FTIR结果表明,在氮气流中焙烧的催化剂,亚铜及氧化铜分布较为均衡,酸性也强于其他样品。CO-FTIR及活性评价结果表明,位于FAU结构中Ⅱ位的亚铜离子,可以与CO形成稳定单羰基络合物,有利于反应的进行。该亚铜离子在氮气焙烧的样品中含量丰富,因此该催化剂具有最高的反应活性。失活研究表明,造成催化剂失活的因素影响程度由大到小排列依次为积碳活性组分流失酸性下降结晶度破坏。在反应过程中,未反应的活化的乙炔气体在分子筛晶粒上溶解、扩散、固化,形成碳颗粒,趋于饱和时,朝着有序的碳纤维的方向生长。热重结果表明,碳纤维的热稳定性要优于前者。
[Abstract]:In order to realize the heterogeneous catalyst for acetylene carbonylation to acrylic acid, a series of bifunctional catalysts supported on active metal components were prepared and their catalytic performance in multiphase reaction system was studied. Based on the research and development experience and basis of nickel-based multiphase catalysts in our laboratory, this paper mainly focuses on the research and development of copper-based multiphase catalysts. In this paper, copper components were supported on Y molecular sieves by liquid phase ion exchange method. At the same time, the structure, composition and acidity of the catalyst were characterized and analyzed by XRD,XPS,ICP-AES,IC,BET,FT-IR,pyridine/CO-IR,NH3-TPD,Raman,TG-DTG and SEM, and the correlation between the catalyst and the activity of the catalyst was studied. the deactivation and regeneration of the most efficient catalyst were studied, and the mechanism of carbon deposition growth was put forward. The characterization results of CuY catalysts prepared by using different copper active component precursors (Cu (NO_3 _ 2, Cubr 鈮，
本文编号：2501496
[Abstract]:In order to realize the heterogeneous catalyst for acetylene carbonylation to acrylic acid, a series of bifunctional catalysts supported on active metal components were prepared and their catalytic performance in multiphase reaction system was studied. Based on the research and development experience and basis of nickel-based multiphase catalysts in our laboratory, this paper mainly focuses on the research and development of copper-based multiphase catalysts. In this paper, copper components were supported on Y molecular sieves by liquid phase ion exchange method. At the same time, the structure, composition and acidity of the catalyst were characterized and analyzed by XRD,XPS,ICP-AES,IC,BET,FT-IR,pyridine/CO-IR,NH3-TPD,Raman,TG-DTG and SEM, and the correlation between the catalyst and the activity of the catalyst was studied. the deactivation and regeneration of the most efficient catalyst were studied, and the mechanism of carbon deposition growth was put forward. The characterization results of CuY catalysts prepared by using different copper active component precursors (Cu (NO_3 _ 2, Cubr 鈮，
本文编号：2501496
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