碱改性γ-Al_2O_3催化剂上羰基硫的低温水解反应 Ⅰ.催化剂活性及补偿效应

CARBONYL SULFIDE HYDROLYSIS ON ALKALIZED Y-A_2O_3 CATALYST AT LOWER TEMPERATURE Ⅰ.CATALYST ACTIVITY AND COMPENSATION EFFECT

以γ-Al_2O_3为载体,用浸渍法负载碱金属和碱土金属氧化物制备了一系列羰基硫水解催化剂。采用微反-色谱联用装置考察了45—100℃低温区内的活性变化规律。结果表明,催化剂活性与金属氧化物组分及含量有着密切关系。在考察各催化剂在不同温度下水解反应速度常数(K)的变化中,发现指前因子(A)与活化能(E)之间存在着补偿效应,活化能增大时指前因子也随之增大。补偿效应参数(K_0)和能量分布指前因子(1/b)均与负载的金属离子半径(d_m)有关。求得了各催化剂的等动力学温度(T),讨论了羰基硫水解反应中存在补偿效应的原因。

A series of A12O3 catalysts impregnated with alkali metal oxides and alkali earth metal oxides for COS hydrolysis was prepared,The activities of the catalysts in a lower temperature range (45-100C) were investigated by means of microreactor-cbromatograpb. It was shown that the catalytic activity was closely related to the oxide and its content. It was also observed that a compensation effect existed by studying the reaction rate constant (K) at various temperatures, j. e. the activation energy (E) increased with the increase of the pro-exponential factor (A), Both compensation effect parameter (K0) and energy distribution exponential factor (1/6) were closely related to the metal ionic radius (dm). The isokinetic temperatures (Ts) of all prepared catalysts were obtained. A possible explanation for the compensation effect in COS hydrolysis was given.