n-Hexadecane hydroisomerization over Pt-HBEA catalysts. Quantification and effect of the intimacy between metal and protonic sites
n-Hexadecane hydroisomerization over Pt-HBEA catalysts. Quantification and effect of the intimacy between metal and protonic sites
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DOI：
10.1016/j.jcat.2013.07.014
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发表时间：
2013-11-01
影响因子：
7.3
通讯作者：
Guisnet, M.
中科院分区：
文献类型：
--
作者：
Batalha, N.;Pinard, L.;Guisnet, M.
正十六烷(n-C-16)在以铂和乙酸乙酯为加氢脱氢组分和酸组分的双功能催化剂上，在220℃和30bar条件下进行了转化。制备了三个系列的催化剂，它们具有不同程度的铂与酸中心的亲和性：系列1中，铂主要位于类12.5微米的HBEA晶团的外表面，系列2和系列3分别是由类70微米的铂-氧化铝和HBEA粒子的组合以及近300微米的铂-氧化铝和HBEA粒子的机械混合形成的。N-C-16临氢异构化的速率和选择性仅由两个参数决定，即金属和酸功能之间的平衡和它们之间的亲和度。两者都很容易量化：第一个是通过可访问的铂和质子中心浓度之间的C-pt/CH+比率，第二个是n(As)，即烯烃中间体在它们在两个铂中心之间扩散时经历的酸步数，可以从初始产物分布中得出。(C)2013 Elsevier Inc.保留所有权利。
n-Hexadecane (n-C-16) transformation was carried out at 220 degrees C and 30 bar over bifunctional catalysts with Pt and HBEA as hydro-dehydrogenating and acid components. Three series of catalysts were prepared, with different levels of proximity between Pt and acid sites: in series 1, Pt was essentially located on the outer surface of HBEA crystal agglomerates of similar to 12.5 mu m, series 2 and 3 resulted from combination of Pt-Al2O3 and HBEA particles of similar to 70 mu m and from mechanical mixture of Pt-Al2O3 and HBEA particles of similar to 300 mu m, respectively. The rate and selectivity of n-C-16 hydroisomerization was shown to be determined by only two parameters, the balance between the metal and acid functions and their degree of intimacy. Both of them were easy to be quantified: the first one by the C-pt/CH+ ratio between the concentrations of accessible Pt and protonic sites, the second one by n(as), the number of acid steps undergone by olefinic intermediates during their diffusion between two Pt sites which can be drawn from the initial product distribution. (C) 2013 Elsevier Inc. All rights reserved.