石油学报（石油加工）
石油學報（石油加工）
석유학보（석유가공）
ACTA PETROLEI SINICA(PETROLEUM PROCESSING SECTION)
2014年
6期
1010-1015
,共6页
丁晓墅%岳川%王淑芳%赵新强%王延吉
丁曉墅%嶽川%王淑芳%趙新彊%王延吉
정효서%악천%왕숙방%조신강%왕연길
负载液膜催化剂%甲醇%碳酸二甲酯%气相合成%高温加压浸渍法
負載液膜催化劑%甲醇%碳痠二甲酯%氣相閤成%高溫加壓浸漬法
부재액막최화제%갑순%탄산이갑지%기상합성%고온가압침지법
supported liquid phase catalyst%methanol%dimethyl carbonate%gas phase synthesis%high temperature and pressure impregnation
制备了新型负载液膜催化剂 PdCl2‐CuCl2‐KOAc‐EG／AC ，并用于甲醇气相氧化羰基化直接合成碳酸二甲酯（DMC），考察了二甘醇、三甘醇和四甘醇及其混合物等不同液膜相，以及制备方法对所制备催化剂在合成DMC反应中催化性能的影响。结果表明，二甘醇作为液膜相，采用高温加压浸渍法制备的催化剂的DMC空时收率比固载型催化剂显著提高。在反应温度160℃、反应压力0.3 MPa、n（CH3 OH）∶ n（CO）∶ n（O2）＝3.6∶2.3∶1、原料气体积空速7100 h－1条件下，DMC空时收率最高可达921 g／（Lcat?h），并且催化剂稳定性也有较大提高。高温加压浸渍法有利于液膜相分散于活性炭孔道中，并保持相对稳定。液膜相的黏度和分子大小是影响负载液膜催化剂反应性能的主要因素。
製備瞭新型負載液膜催化劑 PdCl2‐CuCl2‐KOAc‐EG／AC ，併用于甲醇氣相氧化羰基化直接閤成碳痠二甲酯（DMC），攷察瞭二甘醇、三甘醇和四甘醇及其混閤物等不同液膜相，以及製備方法對所製備催化劑在閤成DMC反應中催化性能的影響。結果錶明，二甘醇作為液膜相，採用高溫加壓浸漬法製備的催化劑的DMC空時收率比固載型催化劑顯著提高。在反應溫度160℃、反應壓力0.3 MPa、n（CH3 OH）∶ n（CO）∶ n（O2）＝3.6∶2.3∶1、原料氣體積空速7100 h－1條件下，DMC空時收率最高可達921 g／（Lcat?h），併且催化劑穩定性也有較大提高。高溫加壓浸漬法有利于液膜相分散于活性炭孔道中，併保持相對穩定。液膜相的黏度和分子大小是影響負載液膜催化劑反應性能的主要因素。
제비료신형부재액막최화제 PdCl2‐CuCl2‐KOAc‐EG／AC ，병용우갑순기상양화탄기화직접합성탄산이갑지（DMC），고찰료이감순、삼감순화사감순급기혼합물등불동액막상，이급제비방법대소제비최화제재합성DMC반응중최화성능적영향。결과표명，이감순작위액막상，채용고온가압침지법제비적최화제적DMC공시수솔비고재형최화제현저제고。재반응온도160℃、반응압력0.3 MPa、n（CH3 OH）∶ n（CO）∶ n（O2）＝3.6∶2.3∶1、원료기체적공속7100 h－1조건하，DMC공시수솔최고가체921 g／（Lcat?h），병차최화제은정성야유교대제고。고온가압침지법유리우액막상분산우활성탄공도중，병보지상대은정。액막상적점도화분자대소시영향부재액막최화제반응성능적주요인소。
The supported liquid phase catalyst was prepared and used in catalytic synthesized dimethyl carbonate(DMC) from gas‐phase oxidative carbonylation of methanol .Diethylene glycol , triethylene glycol and tetraethylene glycol were used as the liquid phases for the supported liquid phase catalyst PdCl2‐CuCl2‐KOAc‐EG/AC ,and the influences of the catalyst preparation conditions on its catalytic performance in synthesis of DMC were investigated .The results showed that PdCl2‐CuCl2‐KOAc‐EG/AC catalyst had the higher yield of DMC than the supported catalyst when diethylene glycol was used as the liquid phase and prepared with high temperature and pressure impregnation .The yield of DMC was reached 921 g/(Lcat?h) at a reaction temperature of 160℃ , reaction pressure of 0.3 MPa ,n(CH3OH)∶ n(CO)∶ n(O2 )=3.6∶2.3∶1 and gas hourly space velocity of 7100 h-1 ,simultaneously ,the catalytic stability of the catalyst was enhanced .Because the viscosity of the liquid phase decreased and the pressure increased in high temperature and pressure impregnation ,the liquid phase was dispersed evenly in the pore and channels of the active carbon and maintained firmly in the supported liquid phase catalyst .The main factors to affect the catalytic performance of the supported liquid phase catalyst were the viscosity and the molecular size of the liquid phase .
