论文部分内容阅读
在无 氧条件下 , Mo/ H Z S M5 催 化剂表 现出良好 的催化甲 烷芳构 化性能. 采用 脉冲 反应, T P S R, T P R , U V Ra m an , X R D 和 B E T 等手段 研究了 反应的诱 导期. B E T 和 X R D 结果表 明,钼物种较好 地分散于 分子筛 的外表面 和孔道内 . T P S R 和 T P R 结果 表明, 在苯 产生 之前 催化 剂上 至少有两种 不同形式 的高价 钼物种被 部分还原 . 参 照 Mo O3/ Al2 O3 的 T P R 结 果,认 为这 两种 高价 钼物种可能 是以多 聚酸盐和 微晶形式 存在的 Mo O3 . U V Ra m an 光谱 表明,催 化剂表面 确实存 在八面体配位的 多聚酸盐 钼物种 ; 而 X R D 没有 检测到 微晶钼物 种的存 在. 脉 冲反应结 果表 明,预 还原 可以缩短反 应诱导 期,而某种 类型积 碳的存在 对缩短 反应诱导 期更为有 利. 根据以上 结果,认 为诱导期是反应 活性相 逐渐形成 的过程, 包括高 价 钼物 种的 部 分还 原 和碳 物种 的 沉积, 而 后者 可能 对 反应更为重 要.
Under anaerobic conditions, the Mo / H ZSM-5 catalyst showed a good catalytic methane aromatization. The induction period of the reaction was studied by means of impulse reaction, T P S R, T P R, U V Raanan, X R D and B E T. The results of B E T and X R D show that molybdenum species are well dispersed on the outer surface of zeolites and in the pores. T P S R and T P R The results show that there are at least two different forms of high valence molybdenum species partially reduced on the catalyst prior to the benzene production. Referring to the T P R results of Mo O3 / Al 2 O 3, it is considered that these two high-priced molybdenum species may be Mo O 3 in the form of polyacid salts and microcrystals. The UV-Raman spectrum shows that there is indeed an octahedrally coordinated polymolybdenum molybdenum species on the catalyst surface; no presence of microcrystalline molybdenum species was detected by XRD. The results of pulse reaction showed that pre-reduction can shorten the induction period, and the existence of some type of carbon deposition is more beneficial to shorten the induction period. Based on the above results, it is considered that the induction period is a process of gradual formation of the reactive phase, including the partial reduction of high-priced molybdenum species and the deposition of carbon species, which may be more important to the reaction.