Na促进的CuCoMn催化剂催化生物质合成气合成高醇(英文)  

Higher Alcohol Synthesis from Bio-Syngas over Na-Promoted CuCoMn Catalyst

作　　者：叶同奇[1] 张朝霞[1] 徐勇[1] 颜世志[1] 朱九方[1] 刘勇 李全新[1] 

机构地区：[1]中国科学技术大学化学物理系,生物质洁净能源安徽省重点实验室,合肥230026 [2]合肥天焱绿色能源开发有限公司,合肥230026

出　　处：《物理化学学报》2011年第6期1493-1500,共8页Acta Physico-Chimica Sinica

基　　金：supported by the National Natural Science Foundation of China (50772107);National Key Basic Research Program of China (973)(2007CB210206);National High-Tech Research and Development Program of China (863) (2009AA05Z435)~~

摘　　要：研究钠促进的CuCoMn催化剂的特性及其在生物质气化合成气合成高醇中的应用. 研究了催化剂中Na含量及合成条件(温度、压力和空速)对生物质基合成气合成高醇性能的影响. 发现CuCoMnNa0.1催化剂较适合高醇合成, 在300 °C以下, 随着温度的上升, 碳转化率增大, 而醇选择性降低. 压力的增加有利于醇的合成,增大空速会明显降低碳转化率, 但醇时空产率则因转换频率的增加而增大. 在所考察的范围内, 醇产率最高达S到ch30u4lz.6-F glo·rkyg)分-1·布h-关1, 其系中. 根C据2+高催醇化(剂C2性-C能6醇与)表占征64分.4析% ,( wN,a 质的量加分入数有)利. 醇于产提物高和生烃物产质物气化均合符成合气AS合F成 (A高nd醇er的so选n-择性和活性元素Cu、Co的分散性. X射线光电子谱(XPS)测试结果显示反应后的催化剂表面上, Cu以Cu+和Cu0的混合形式存在, 而 Co 则是 Co2+/Co3+和 Co0的混合物. 增加 Na 的含量, Cu0/Cu+比率和 Co0的强度均随之减小.Na-promoted CuCoMn catalysts were successfully applied to the highly efficient production of higher alcohols from bio-syngas, which was derived from biomass gasification. The influence of Na content and synthesis conditions （temperature, pressure, and gas hourly space velocity （GHSV）） on higher alcohol synthesis was investigated. The CuCoMnNa0.1 catalyst gave the best performance for higher alcohol synthesis. Carbon conversion increased significantly with an increase in temperature at lower than 300 °C but alcohol selectivity showed an opposite trend. A higher pressure was found to be beneficial for higher alcohol synthesis. Increasing the GHSV reduced carbon conversion but increased the yield of higher alcohols. The maximum higher alcohol yield that was derived from bio-syngas was 304.6 g·kg-1·h-1 with the C2＋ alcohols （C2-C6 higher alcohols） of 64.4% （w, mass fraction） under the conditions used. The distributions of the alcohols and the hydrocarbons were consistent with Anderson-Schulz-Flory （ASF） plots. Adding Na to the CuCoMn catalysts led to an increase in the selectivity toward the higher alcohols and promoted the dispersion of the active elements, copper and cobalt. X-ray photoelectron spectroscopy （XPS） results suggested that Cu was present as a mixture of Cu＋ and Cu0 on the catalyst′s surface after use and Co was present as a mixture of Co2＋/Co3＋ and Co0. With an increase in sodium addition the Cu0/Cu＋ ratio and the Co0 intensity both decreased.

关 键 词：生物质 生物质合成气 高醇 ASF分布 CuCoMnNa催化剂 

分 类 号：TQ223.12[化学工程—有机化工]