纳米Pd/AC催化顺酐“一锅法”水相合成丁二酸  

Hydrogenation of Maleic Anhydride to Succinic Acid in Aqueous Medium over Nano-Pd/AC Catalyst by One-Pot Method

作　　者：刘娜[1] 荣泽明[1] 王勇[1] 郭启迪[1] 吕欣怡[1] 王伊凡[1] 

机构地区：[1]大连理工大学化工与环境生命学部精细化工国家重点实验室,辽宁大连116024

出　　处：《石油化工》2012年第1期66-71,共6页Petrochemical Technology

基　　金：辽宁省教育厅2010年度高等学校科研项目计划(LT2010021);大连理工大学基本科研业务费专项资金项目(DUT10RC(3)107)

摘　　要：将改性骨架镍催化剂、贵金属负载型催化剂用于"一锅法"水相顺酐催化加氢合成丁二酸,考察了催化剂种类、反应温度、反应压力、顺酐用量及催化剂用量对该反应的影响,并用XRD和TEM法对反应前后催化剂的微观结构进行了表征。结果表明,由胶体溶液法制备的负载型纳米Pd/AC(AC为活性炭)催化剂的性能最好。在353 K、1.0 MPa、顺酐1.96 g、水20mL、2%(w)Pd/AC催化剂0.020 g的优化条件下反应177 min时,顺酐转化率达100.0%,丁二酸选择性达99.8%。Pd/AC催化剂的稳定性实验结果显示,该催化剂连续使用10次后仍能维持较高的活性和选择性。新鲜Pd/AC催化剂中Pd颗粒分散均匀,粒径为1～4 nm;连续使用10次后Pd/AC催化剂部分发生团聚,但仍存在大量的纳米级Pd晶粒,使反应稳定进行。A modified skeletal nickel catalyst and supported noble metal catalysts were used in hydrogenation of maleic anhydride into succinic acid in aqueous medium by one-pot method. The effects of catalyst type, reaction temperature, reaction pressure, maleic anhydride dosage and catalyst dosage on the hydrogenation were investigated. The microstructures of both the fresh and the used catalysts were characterized by means of XRD and TEM. The results showed that the catalytic performance of nano-palladium/active carbon （nano-Pd/AC） prepared by colloidal solution method was excellent. Under the optimized reaction conditions of 353 K, 1.0 MPa, maleic anhydride 1.96 g, H20 dosage 20 mL, Pd/AC catalyst with 2%（w） Pd 0.020 g and 177 min, the conversion of maleic anhydride and the selectivity to succinic acid reached 100.0% and 99.8%, respectively. The catalyst exhibited good activity and selectivity after it was reused for ten times. XRD and TEM characterization indicated that Pd nano-particles on the fresh catalyst were in a good dispersion state and their sizes were between 1-4 nm. The partial aggregation of the Pd nanoparticles on the used catalysts was observed, but because of the existence of many other Pd nano-particles on the catalyst, the hydrogenation could proceed stably.

关 键 词：顺酐 丁二酸 钯/活性炭催化剂 加氢 

分 类 号：TQ032.41[化学工程]