物理化学学报 >> 2017, Vol. 33 >> Issue (8): 1672-1680.doi: 10.3866/PKU.WHXB201704143

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Cu含量对以水滑石为前驱体的Cu/Co/Mn/Al催化剂高级醇合成性能的影响

廖珮懿1,2,张辰1,2,张丽君1,杨彦章2,钟良枢2,郭晓亚1,王慧2,*(),孙予罕2,*()   

  1. 1 上海大学环境与化学工程学院,上海200444
    2 中国科学院上海高等研究院,上海201210
  • 收稿日期:2016-12-28 发布日期:2017-06-14
  • 通讯作者: 王慧,孙予罕 E-mail:wanghh@sari.ac.cn;yhsun@sari.ac.cn
  • 基金资助:
    国家自然科学基金(21403278);神华集团有限责任公司;山西潞安矿业(集团)有限责任公司;荷兰皇家壳牌集团

Influences of Cu Content on the Cu/Co/Mn/Al Catalysts Derived from Hydrotalcite-Like Precursors for Higher Alcohols Synthesis via Syngas

Pei-Yi LIAO1,2,Chen ZHANG1,2,Li-Jun ZHANG1,Yan-Zhang YANG2,Liang-Shu ZHONG2,Xiao-Ya GUO1,Hui WANG2,*(),Yu-Han SUN2,*()   

  1. 1 School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P. R. China
    2 Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, P. R. China
  • Received:2016-12-28 Published:2017-06-14
  • Contact: Hui WANG,Yu-Han SUN E-mail:wanghh@sari.ac.cn;yhsun@sari.ac.cn
  • Supported by:
    The project was supported by the National Natural Science Foundation of China(21403278);China Shenhua Coal to Liquid;Chemical Company Limited, Shanxi Lu?an Coal Corporation Limited;Shell Global Solutions International B. V

摘要:

采用共沉淀法制备了一系列不同铜钴摩尔比(0,0.1,0.5,1.0,2.0)的Cu/Co/Mn/Al层状结构催化剂并考察了其在合成气制混合醇反应中的催化性能,采用N2物理吸脱附、电感耦合等离子体原子发射光谱法(ICP-AES)、X射线衍射(XRD)、扫描电子显微镜(SEM)、氢气程序升温还原(H2-TPR),热重分析(TG)和高分辨透射电子显微镜(HRTEM)等对催化剂进行了表征分析。结果表明,适当的铜钴摩尔比可以增大催化剂的比表面积,提高催化剂的还原性能,并能形成较规整的层状结构从而提供更均一分散的合成醇活性位,从而提高催化活性和醇选择性。当铜钴摩尔比为0.5时,得到最高的醇时空产率(STY)和醇质量选择性,分别为0.071 g·g-1·h-1和35.9%。

关键词: 高级醇合成, 水滑石前驱体, Cu/Co/Mn/Al催化剂, 铜钴摩尔比, 合成气转化

Abstract:

A series of Cu/Co/Mn/Al catalysts derived from hydrotalcite precursors with different Cu/Co molar ratios (0, 0.1, 0.5, 1.0, and 2.0) were prepared and used for the synthesis of higher alcohols from syngas. N2 physical adsorption desorption, inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray diffraction (XRD), scanning electron microscopy (SEM), hydrogen temperature-programmed reduction (H2-TPR), thermogravimetry (TG), and high-resolution transmission electron microscopy (HRTEM) techniques were employed to investigate the physical and chemical properties of the Cu/Co/Mn/Al catalysts. The results show that the optimum Cu content can increase specific surface area, improve reducibility, and form regular layered structure to provide more uniform distribution of active sites, thereby enhancing catalytic activity and alcohol selectivity. When the Cu/Co molar ratio was 0.5, the yield of alcohol and the alcohol selectivity reached the maximum values of 0.071 g·g-1·h-1 and 35.9%, respectively.

Key words: Higher alcohols synthesis, Layered-double hydroxide, Cu/Co/Mn/Al catalyst, Cu/Co molar ratio, Syngas conversion

MSC2000: 

  • O643