Pd对Zr-Mn-K催化CO加氢合成甲醇与异丁醇的影响  

Effect of Pd on Catalytic Performance of Zr-Mn-K Catalyst for CO Hydrogenation to Methanol and Isobutanol

作　　者：何代平[1] 丁云杰[1] 尹红梅[1] 朱何俊[1] 熊健民[1] 罗洪源[1] 

机构地区：[1]中国科学院大连化学物理研究所,辽宁大连116023

出　　处：《催化学报》2003年第9期658-662,共5页

基　　金：中国科学院创新基金资助课题 (KGCX2 3 0 2 0 1)

摘　　要：考察了添加Pd对Zr Mn K催化CO加氢合成甲醇与异丁醇的影响 .与Zr Mn K催化剂相比 ,Pd/Zr Mn K催化剂的催化活性及异丁醇选择性明显升高 .在SV =10 0 0 0h-1,p =8 0MPa和T =6 73K的反应条件下 ,1 5 %Pd/Zr Mn K催化剂上醇的时空收率由原来的 12 2 8升高到 2 32 6 g/ (kg·h) ,异丁醇的选择性由原来的 15 5 %升高到 2 1 7% .当Pd的添加量大于1 5 %时 ,催化剂的活性及异丁醇选择性开始下降 .H2 和CO吸附实验结果表明 ,Pd/Zr Mn K催化剂表面维持有较高的H2 和CO吸附量 ,有利于甲醇与异丁醇生成速率的提高 .当Pd的添加量超过 1 5 %时 ,Pd的分散度降低 ,粒径变大 ,吸附H2 和CO的量减少 。The influence of Pd on the catalytic performance of Zr Mn K catalyst for the selective synthesis of methanol and isobutanol from syngas was investigated. Compared with Zr Mn K catalyst, the Pd promoted Zr Mn K catalyst significantly improved the reaction activity. Under the reaction conditions of SV= 10?000 h -1 , p =8 0 MPa and T =673 K, the space time yield of alcohols increased greatly from 122 8 to 232 6 g/(kg·h) when 1 5%Pd (Pd(NO 3) 2 as precursor) was addedd into the Zr Mn K catalyst, and the selectivity for isobutanol increased from 15 5% to 21 7%. However, the catalytic activity and selectivity for isobutanol greatly decreased when the Pd loading exceeded 1 5%. The influence of the reaction conditions was also investigated. The reaction conditions of 15?000 h -1 , higher pressure and 673 K are optimum for isobutanol synthesis from CO hydrogenation. The chemisorption of H 2 and CO on Zr Mn K and Pd/Zr Mn K catalysts revealed that H 2 and CO uptakes on Pd/Zr Mn K catalyst are higher than those on Zr Mn K catalyst. The higher H 2 and CO uptakes on Pd/Zr Mn K catalyst would be in favor of enhancement in the rate of methanol and isobutanol synthesis. The uptakes of H 2 and CO decreased with Pd loading in excess of 1 5%, so that the space time yield of methanol and isobutanol decreased.

关 键 词：钯 锆 锰 钾 一氧化碳 加氢 甲醇 异丁醇 

分 类 号：O643.3[理学—物理化学]