CAJ | 학술논문

采用Cu-K/Al2 O3催化剂，在固定床积分反应器上进行溴甲烷合成二甲醚的动力学实验，反应温度（463.15~523.15）K条件下，得出主反应的宏观动力学方程：r=1.1+2.8×10-3 T-4.4exp（-21.5RT ）pCH3Br，主反应的活化能约为21.5 kJ·mol-1。对主反应宏观动力学方程进行统计检验，结果表明，在给定99%的置信度下，方程显著、可信。失活前后的XRD表征结果表明，催化剂晶相由CuO转变为CuBr2是导致催化剂失活的主要原因。采用独立失活机理描述催化剂失活速率方程，通过回归得到各项参数，建立了适用于Cu-K/Al2 O3催化剂上溴甲烷合成二甲醚的失活动力学方程：r=[-1.1+2.8×10-3T-4.4exp（-21.5RT ）pCH3Br]×exp（-2.1×10-3t）。
채용Cu-K/Al2 O3최화제，재고정상적분반응기상진행추갑완합성이갑미적동역학실험，반응온도（463.15~523.15）K조건하，득출주반응적굉관동역학방정：r=1.1+2.8×10-3 T-4.4exp（-21.5RT ）pCH3Br，주반응적활화능약위21.5 kJ·mol-1。대주반응굉관동역학방정진행통계검험，결과표명，재급정99%적치신도하，방정현저、가신。실활전후적XRD표정결과표명，최화제정상유CuO전변위CuBr2시도치최화제실활적주요원인。채용독립실활궤리묘술최화제실활속솔방정，통과회귀득도각항삼수，건립료괄용우Cu-K/Al2 O3최화제상추갑완합성이갑미적실활동역학방정：r=[-1.1+2.8×10-3T-4.4exp（-21.5RT ）pCH3Br]×exp（-2.1×10-3t）。
Based on the kinetics experiment carried out in the integral fixed bed reactor and under the condition of reaction temperature(463. 15-523. 15)K,the macro kinetic equation of methyl bromide to dimethyl ether over Cu-K/Al2O3 catalyst was obtained as follows:r=1. 1+2.8 ×10-3T-4.4exp(-21.5RT ) pCH3Br . The activation energy of the main reaction was about 21. 5 kJ·mol-1 . The results of statistical validation showedthatthemacrokineticequationwassignificantandcredibleatthe99%belief.TheresultsofXRD characterization indicated that the crystal phase transformation of the catalyst from CuO to CuBr2 was the main reason for its deactivation. According to independent deactivation mechanism,the deactivation kinetic equation for methyl bromide to dimethyl ether over Cu-K/Al2 O3 catalyst was established as follows:r=[ -1.1+2.8 ×10 -3T-4.4exp( -21.5RT )pCH3Br]×exp( -2.1 ×10 -3t).