反应氛围对RBS-1分子筛催化剂上气相Beckmann重排反应的影响

THE EFFECT OF REACTION ATMOSPHERES ON THE VAPOR PHASE BECKMANN REARRANGEMENT OVER RBS-1 MOLECULAR SIEVE CATALYST

在常压连续流动固定床反应装置上，考察了反应温度、环己酮肟质量空速（MHSV）、溶剂种类、环己酮肟浓度、载气流量、水的质量分数等反应条件或反应氛围对环己酮肟气相Beckmann重排反应的影响。结果表明，低碳醇适宜作反应溶剂；环己酮肟浓度和载气流量对反应性能有较大影响；反应物料中加入少量水可降低催化剂的失活速率，并可改善己内酰胺的选择性。在微型固定床反应装置上得到的优化反应工艺条件为：催化剂用量0．375g，反应压力101．3kPa，反应温度653～663K，反应物溶剂为乙醇，环己酮肟的MHSV为1～2h^-1，环己酮肟的质量分数为33％～44％，N2载气流量为30-45ml／min。

The vapor phase Beckmann rearrangement of cyclohexanone oxime（CHO）over RBS-1 catalyst was carried out in a continuous flow fixed bed reactor under atmosphere pressure. The influences of reaction temperature, MHSV of CHO, CHO concerntration, mass fraction of water, various solvents and flow rate of carrier gas on the vapor phase Beckmann rearrangement of CHO were observed. The low carbon alcohols were the most effective solvent for the Beckmann reaction. The CHO concerntration and flow rate of carrier gas influenced the catalytic activity when the MHSV of CHO was set, but the selectivity for lactam was almost unchanged. Addition of water in the reaction mixture could minimize the catalyst deactivation and improve the lactam selectivity. The optimum reaction conditions on the micro bed reactor were as follows： catalyst of 0.375 g,101.3 kPa, 653-663 K, CHO MHSV of 1-2 h^-1, ethanol as solvent, 33%-34% of CHO mass fraction,30-45 ml/min of flow rate of N2 carrier gas.