锰和镧改性Cu/ZrO_2合成甲醇催化剂的结构及催化性能  

Structure and Catalytic Performance of Mn-and La-Modified Cu/ZrO_2 Catalysts for Methanol Synthesis

作　　者：林明桂[1,2] 杨成[3] 吴贵升[3] 魏伟[3] 李文怀[3] 单永奎[1] 孙予罕[3] 何鸣元[1] 

机构地区：[1]华东师范大学化学系 [2]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [3]中国科学院山西煤炭化学研究所煤转化国家重点实验室

出　　处：《催化学报》2004年第7期591-595,共5页

基　　金：上海市重大科技项目;国家重点基础研究发展规划项目 (G19990 2 2 40 4)

摘　　要：考察了锰和镧助剂对Cu/ZrO2 催化剂上CO加氢合成甲醇反应性能的影响 ,并通过BET ,XRD ,TPR ,H2 TPD和CO TPD等手段对催化剂的结构及吸附 脱附性能进行了研究 .结果表明 ,锰和镧两种助剂均能有效地提高催化剂的活性 ,同时引入两种助剂时可使催化剂的活性进一步提高 ,表现出较强的协同效应 .一方面 ,锰的加入可使催化剂各组分的相互作用增强 ,特别是铜锰复合物的形成可有效地促进活性组分的分散 ,防止催化剂的烧结 ;另一方面 ,镧助剂的引入进一步增强了铜锆在界面的相互作用 ,稳定了催化剂的活性中心 。Cu/ZrO 2 is well known as a good catalyst for methanol synthesis from CO/CO 2 hydrogenation. In order to improve its catalytic performance, the effects of the addition of Mn and La promoters to Cu/ZrO 2 catalyst were investigated. The structure and adsorptive properties of the catalysts were characterized by BET, XRD, TPR, H 2 TPD and CO TPD techniques. Both the promoters possessed separately the capacity of improving the catalyst activity with the La component being better dopant. The catalyst activity was remarkably improved by the addition of Mn and La together, and the space time yield of methanol reached 1 128 g/(ml·h) under the mild reaction conditions (GHSV= 3?000 h -1 , p =6 0 MPa, θ =250 ℃). Combined with the characterization results, a synergistic effect in La and Mn co modified Cu/ZrO 2 catalyst was suggested. On the one hand, the interaction of Cu and Mn enhanced the dispersion of the active component owing to the formation of CuMnO x composite, which prevented active phase Cu from crystallizing and sintering. On the other hand, the presence of La effectively increased the strength of the interaction between Cu and ZrO 2, and therefore stabilized the active center of the catalyst, and facilitated the spillover between Cu and ZrO 2.

关 键 词：铜 氧化锆 负载型催化剂 锰 镧 助剂 协同作用 甲醇合成 

分 类 号：O643[理学—物理化学]