磷酸锆类层柱催化剂的制备、表征及其催化甲醇氧化羰基化反应性能

PREPARATION AND CHARACTERIZATION OF LAYERED PILLARED ZIRCONIUM PHOSPHATE AND ITS CATALYTIC PERFORMANCE FOR OXIDATIVE CARBONYLATION OF METHANOL

以层 状 α磷酸 锆为插层 主体，采 用高温 固相 离子 交换 插层 法制 备了 Ｃｕ２ ＋ ， Ｋ ＋ 柱 撑 的磷酸锆类 层柱催化 剂，并用 Ｘ Ｒ Ｄ， Ｉ Ｒ 和 Ｔ Ｇ 等方 法对 其进 行了 表征 ． 结 果 表明 ，金 属离 子柱 撑 的 α磷酸锆 类层柱催 化剂的 层间距由 原来的０ ７６ ｎ ｍ 扩 撑至０８１ ｎ ｍ ， 结 晶度 有所 下降 ． 通 过甲 醇氧化羰基 化液相法 制备碳 酸二甲酯 反应，考 察了磷 酸锆 类层 柱催 化剂 的催 化性 能． 在一 定的 反 应条件下，甲 醇转化 率可达１６ ７ ％ ， 碳酸 二甲酯选 择性可达 ５７ ％ ， 而 且催化 剂用 量少， 结构 稳定， 对设备腐蚀

Cupric and potassium ions layered pillared zirconium phosphate (Ⅰ) was prepared by the intercalation of Cu 2+ and K +. It was shown that the interlayer distance increased from 0 76 nm to 0 81 nm and the crystallinity went down after Cu 2+ and K + were intercalated into the layers. The influence of reaction conditions on its catalytic performance in oxidative carbonylation of methanol to dimethyl carbonate (DMC) was studied. Under the best reaction conditions, the methanol conversion was 16 7% and the selectivity for DMC was 57%. Compared with the traditional catalyst CuCl, (I) has advantages in activity, thermostability and corrosion to the equipment, but its selectivity for DMC was lower.