Mn和Zr助剂对介孔碳负载钴基催化剂费托合成反应性能的影响

张庆玲; 郭荷芹; 侯博; 王俊刚; 李德宝; 贾丽涛

Mn和Zr助剂对介孔碳负载钴基催化剂费托合成反应性能的影响

张庆玲^{1, 2},
郭荷芹¹,
侯博¹,
王俊刚¹,
李德宝¹,
贾丽涛^1, ,

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

基金项目:

国家自然科学基金 21273265

国家自然科学基金 21503252

中国科学院战略性先导科技专项“低阶煤清洁高效梯级利用关键技术与示范” XDA07070700

山西省煤基重点科技攻关项目 MH2014-13

山西省基础研究计划项目 2014021014-6

山西省基础研究计划项目 201601D021044

详细信息

通讯作者:
贾丽涛, Tel/Fax:0351-4040466, 0351-4041153, E-mail:jialitao910@163.com

中图分类号: O643
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- 文章访问数: 99
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- 被引次数: 0
出版历程
- 收稿日期: 2017-03-03
- 修回日期: 2017-04-20
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-06-10

Effects of Mn and Zr promoters on the performance of ordered mesoporous carbon supported Co catalyst in Fischer-Tropsch synthesis

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Funds:

the National Natural Science Foundation of China 21273265

the National Natural Science Foundation of China 21503252

the "Strategic Priority Research Program"Demonstration of Key Technologies for Clean and Efficient Utilization of Low-rank Coal XDA07070700

the Coal Base Key Technologies R & D Program of ShanXi Province MH2014-13

the ShanXi Provincial Research Foundation for Basic Research 2014021014-6

the ShanXi Provincial Research Foundation for Basic Research 201601D021044

摘要

摘要: 采用浸渍法制备了Mn和Zr改性的介孔碳负载钴基催化剂，采用X射线衍射（XRD）、比表面积测定、H₂程序升温还原（H₂-TPR）、H₂/CO程序升温脱附（TPD）及X射线光电子能谱（XPS）等手段对催化剂的物化性质进行了表征，采用固定床反应器对其F-T反应性能进行了研究。结果表明，Mn或Zr助剂的添加均降低了CH₄的选择性。其中，Mn助剂的添加提高了C_2-4的选择性，提高了烯烷比，而Zr的添加提高了钴物种的分散度，增加了反应活性位点，显著提高了钴基催化剂的F-T反应活性和C₅₊选择性。
- 费托合成 /
- 钴基催化剂 /
- 介孔碳 /
- 锰助剂 /
- 锆助剂
Abstract: Cobalt-based catalysts supported on ordered mesoporous carbon (Co/OMC) were modified with Mn and Zr promoters by the co-impregnation method. The cobalt-based catalysts were characterized by XRD, N₂ sorption, H₂-TPR, H₂/CO-TPD and XPS; the promoting effects of Mn and Zr on the catalytic performance of Co/OMC in Fischer-Tropsch synthesis (FTS) were investigated in a fixed-bed reactor. The results indicate that the addition of either Mn or Zr can greatly reduce the selectivity to CH₄ for FTS over Co/OMC. Moreover, Mn as a promoter can enhance the selectivity to C_2-4 hydrocarbons and the olefin/paraffin ratio, whereas Zr promotes the dispersion of cobalt species and increases the number of active Co sites, leading to a significant increase in the FTS activity and selectivity to C₅₊ hydrocarbons.
- Fischer-Tropsch synthesis /
- cobalt-based catalyst /
- mesoporous carbon /
- Mn promoter /
- Zr promoter

HTML全文

图 1 催化剂的XRD谱图

Figure 1 XRD patterns of various catalysts

(a): fresh catalysts; (b): reduced catalysts

下载: 全尺寸图片幻灯片

图 2 催化剂的Co 2p XPS谱图

Figure 2 Co 2p XPS spectra of various catalysts

(a): fresh catalysts; (b): reduced catalysts

下载: 全尺寸图片幻灯片

图 3 催化剂的H₂-TPR谱图

Figure 3 H₂-TPR profiles of various catalysts

下载: 全尺寸图片幻灯片

图 4 催化剂的H₂-TPD谱图

Figure 4 H₂-TPD profiles of various catalysts

下载: 全尺寸图片幻灯片

图 5 催化剂的CO-TPD谱图

Figure 5 CO-TPD profiles of various catalysts

下载: 全尺寸图片幻灯片

表 1 催化剂的织构参数和晶粒粒径

Table 1 Texture parameters and Co/CoO particle size of various catalysts

表 2 催化剂的表面组成

Table 2 Surface compositions of various catalysts

表 3 催化剂的反应性能

Table 3 Catalytic performance of various catalysts in FTS

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