自然科学版
陕西师范大学学报(自然科学版)
合成气定向催化转化科学与技术专题
K对Cu/Zn/La/ZrO2催化剂上CO加氢制备异丁醇的影响
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武应全1, 张涛1, 张俊峰1, 王立言1,2, 解红娟1,杨国辉1, 谭猗生1,3*
(1 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;2中国科学院大学,北京 100049;3 中国科学院山西煤炭化学研究所, 国家煤基合成工程技术研究中心,山西 太原 030001)
谭猗生,男,研究员,博士生导师,主要从事多相催化方面的研究。E-mail: tan@sxicc.ac.cn
摘要:
采用共沉淀法制备了碱金属K改性Cu/Zn/La/ZrO2催化剂,在固定床反应器上分析了其在合成气制异丁醇反应中的催化性能,利用BET、XRD、CO2-TPD、NH3-TPD及 CO-TPD表征技术,研究了K助剂的添加和反应温度对催化剂性能的影响。结果发现:K助剂不仅对催化剂结构及表面性质影响较大,同时对异丁醇合成活性也有明显影响。K改性导致催化剂各活性组分分散性变差,催化剂晶粒增大,CuO还原温度升高。但K促进了催化剂表面弱酸酸量及弱碱碱量的增加,催化剂上弱酸酸量、弱碱碱量分别与CO吸附性能、总醇时空收率有较好的顺变关系。结果表明:适宜的弱酸、弱碱中心有利于提高总醇的时空收率和总醇中异丁醇的选择性。
关键词:
碱金属; Cu/Zn/La/ZrO2催化剂; 合成气; 异丁醇
收稿日期:
2018-10-31
中图分类号:
O643.36
文献标识码:
A
文章编号:
1672-4291(2019)01-0052-08
基金项目:
国家自然科学基金(21573269)
Doi:
Effect of potassium on CO hydrogenation to isobutanol over Cu/Zn/La/ZrO2 catalyst
WU Yingquan1, ZHANG Tao1, ZHANG Junfeng1, WANG Liyan1,2,XIE Hongjuan1, YANG Guohui1, TAN Yisheng1,3*
(1 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China;2 University of the Chinese Academy of Sciences, Beijing 100049, China;3 National Engineering Research Center for Coal-Based Synthesis, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China)
Abstract:
The alkaline promoter K modified Cu/Zn/La/ZrO2 catalysts were prepared using the coprecipitation method, and used for the synthesis of isobutanol from syngas in a fixed bed reactor. The effects of K promoter and reaction temperature on the catalytic performance were investigated in combination of BET, XRD, CO2-TPD, NH3-TPD and CO-TPD characterizations. The results indicated that addition of K inhibited the dispersion of each component, leading to the larger particle size. Meanwhile, reduction peaks of CuO shifted to the higher temperature. However, addition of K led to an increase in the amount of weak acidic sites and weak base sites, which have remarkably close relationships with CO adsorption and space-time yield (STY) of alcohol. Moderate weak acid and base sites were beneficial to improve the STY of total alcohols and the selectivity of isobutanol in total alcohols.
KeyWords:
alkaline metal; Cu/Zn/La/ZrO2 catalyst; syngas; isobutanol