水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性

马利海; 张建利; 范素兵; 赵天生

水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性

宁夏大学省部共建天然气转化国家重点实验室培育基地, 宁夏银川 750021

基金项目: 国家重点基础研究发展规划(973计划, 2012CB723106)。

详细信息

通讯作者:
赵天生,E-mail:zhaots@nxu.edu.cn;张建利,E-mail:zhangjl@nxu.edu.cn;Fax:0951-2062323。

中图分类号: O643
计量
- 文章访问数: 1358
- HTML全文浏览量: 30
- PDF下载量: 856
- 被引次数: 0
出版历程
- 收稿日期: 2013-02-28
- 修回日期: 2013-04-14
- 刊出日期: 2013-11-30

Preparation of Fe-Mn catalyst by hydrothermal method and its catalytic activity for the synthesis of light olefins from CO hydrogenation

State Key Laboratory Cultivation Base of Natural Gas Conversion, Ningxia University, Yinchuan 750021, China

摘要

摘要: 以水热合成法制备了K原位改性的Fe-Mn催化剂,考察了其CO加氢合成低碳烯烃催化活性。采用SEM、TEM、XRD、H₂-TPR和FT-IR等手段对催化剂进行了表征。结果表明,制备的催化剂前驱体呈50~70 nm的球形颗粒,表面富含羰基和羟基,物相组成以Fe₃O₄为主,用于反应后有Fe₅C₂和MnCO₃相生成。与共沉淀法制备催化剂相比,在设定的反应条件下,不同K含量改性的催化剂均具有较高的活性,以原料配比Fe:Mn:C₆:K=3:1:5:0.10的催化剂性能最佳,CO转化率达95.02%,总低碳烯烃收率为62.86 g/m³(H₂+CO),CH₄和CO₂选择性分别为13.88%和13.98%。
- Fe-Mn催化剂 /
- 水热法 /
- CO加氢 /
- 低碳烯烃
Abstract: A series of potassium modified Fe-Mn catalysts were prepared by hydrothermal method and applied to the catalytic synthesis of light olefins from CO hydrogenation. The catalyst samples were characterized by SEM, TEM, XRD, H₂-TPR and FT-IR techniques. Results showed that the prepared sample particles were spherical with 50~70 nm size and the carbonyl and hydroxy groups were observed on their surfaces. The bulk composition was mainly Fe₃O₄ before the reaction. Fe₅C₂ and MnCO₃ were formed after the reaction. The prepared samples showed high activity and olefin selectivity under the given reaction conditions. Using the sample S₃ (Fe:Mn:C₆:K=3:1:5:0.10), the CO conversion and the olefin productivity reached 95.02% and 62.86 g/m³ (H₂+CO), respectively. Compared with the catalyst prepared with co-precipitation method, the S₃ catalyst had lower CH₄ selectivity(13.88%) and CO₂ selectivity(13.98%).
- Fe-Mn catalyst /
- hydrothermal method /
- CO hydrogenation /
- light olefins

HTML全文

参考文献(16)

董丽, 杨学萍. 合成气直接制低碳烯烃技术发展前景[J]. 石油化工, 2012, 4(10): 1201-1206. (DONG Li, YANG Xue-ping. New advances in direct production of light olefins from syngas[J]. Petrochemical Technology, 2012, 4(10): 1201-1206.)

ZHANG Q H, KANG J C, WANG Y. Development of novel catalysts for Fischer-Tropsch synthesis: Tuning the product selectivity[J]. ChemCatChem, 2010, 2(9): 1030-1058.

RAJE A P, DAVIS B H. Fischer-Tropsch synthesis over iron-based catalysts in a slurry reactor reaction rates, selectivities and implications for improving hydrocarbon productivity[J]. Catal Today, 1997, 36(6): 335-345.

YANG Y, XIANG H W, ZHANG Y L. A highly active and stable Fe-Mn catalyst for slurry Fischer-Tropsch synthesis[J]. Catal Today, 2005, 106(12): 170-175.

ZHOU J, CHU W, ZHANG H, XU H, ZHANG T. Effect of Fe content on FeMn catalysts for light alkenes synthesis[J]. Nat Gas Chem Ind, 2008, 2(3): 315-318.

YANG Y, XIANG H W, XU Y Y, LI Y W. Effect of potassium promoter on precipitated iron-manganese catalyst for Fischer-Tropsch synthesis[J]. Appl Catal A: Gen, 2004, 266(2): 181-194.

NING W S, KOIZUMI N, YAMADA M. Improvement of promoters on the Fischer Tropsch activity of mechanically mixed Fe catalysts[J]. Catal Commun, 2007, 8(3): 275-278.

张敬畅, 曹维良, 单伟力, 李梦波. 激光热解法制备铁基超微粒子催化剂及催化性能评价[J]. 催化学报, 1998, 19(1): 63-66. (ZHANG Jing-chang, CAO Wei-liang, SHAN Wei-li, LI Meng-bo. Preparation and characterization of Fe/ AC catalysts for synthesis of light olefins via carbon monoxide hydrogenation[J]. Chinese Journal of Catalysis, 1998, 19(1): 63-66.)

GALVIS H M T, BITTER J H, KHARE C B, RUITENBEEK M, DUGULAN A L, JONG K P. Supported iron nanoparticles as catalysts for sustainable production of lower olefins[J]. Science, 2012, 335(2): 835-838.

禹国宾. 新型催化材料的制备及其在费托合成中的应用[D]. 复旦大学, 2009. (Yu Guo-bin. The preparation of a new catalytic material applying for F-T Synthesis[D]. Fudan University, 2009.)

XU L, DU J, LI P, QIAN Y. In situ synthesis, magnetic property, and formation mechanism of Fe₃O₄ particles encapsulated in ID Bamboo-Shaped carbon microtubes[J]. J Phys Chem B, 2006, 110(5): 3871-3875.

付伯承. 碳包覆纳米四氧化三铁颗粒的合成与结构研究[D]. 北京化工大学, 2010. (FU Bo-cheng. Preparation and structure of carbon-encapsulated Fe₃O₄ nanoparticles[D]. Beijing University of Chemical Technology, 2010.)

SUN X M, LIU J F, LI Y D. Use of carbonaceous polysaccharide microspheres as templates for fabricating metal oxide hollow spheres[J]. Chem Eur J, 2006, 12(7): 2039-2047.

BUKUR D B, LANG X S, DING Y J. Pretreatment effect studies with a precipitated iron Fischer-Tropsch catalyst in a slurry reactor[J]. Appl Catal A: Gen, 1999, 186(1/2): 255-275.

李先国, 王琴, 钟炳, 彭少逸, 马玉刚, 吴东. 铁基超细粒子催化剂的F-T反应性能研究I. Fe-Mn催化剂的反应性能、活性相结构及锰的作用[J]. 燃料化学学报, 1993, 21(4): 344-349. (LI Xian-guo, WANG Qin, ZHONG Bing, PENG Shao-yi, MA Yu-gang, WU Dong. Studies on the F-T performance of iron based ultrafing catalysts I: Performance of Fe-Mn catalyst, active phases and role of Mn[J]. Journal of Fuel Chemistry and Technology, 1993, 21(4): 344-349.)

LEITH I R, HOWDEN M G. Temperature-programmed reduction of mixed iron-manganese oxide catalysts in hydrogen and carbon monoxide[J]. Appl Catal, 1988, 27(2): 75-92.

施引文献

资源附件(0)

访问统计

点击查看大图

计量

文章访问数: 1358
HTML全文浏览量: 30
PDF下载量: 856
被引次数: 0

姓名
邮箱
手机号码
标题
留言内容
验证码

留言板

水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性

通讯作者:
赵天生,E-mail:zhaots@nxu.edu.cn;张建利,E-mail:zhangjl@nxu.edu.cn;Fax:0951-2062323。

计量

Preparation of Fe-Mn catalyst by hydrothermal method and its catalytic activity for the synthesis of light olefins from CO hydrogenation

计量

目录

2023年《燃料化学学报（中英文）》评优结果公布！

留言板

水热法Fe-Mn催化剂制备及其合成气制低碳烯烃催化活性

通讯作者: 赵天生,E-mail:zhaots@nxu.edu.cn;张建利,E-mail:zhangjl@nxu.edu.cn;Fax:0951-2062323。

计量

出版历程

Preparation of Fe-Mn catalyst by hydrothermal method and its catalytic activity for the synthesis of light olefins from CO hydrogenation

计量

出版历程

目录

2023年《燃料化学学报（中英文）》评优结果公布！

通讯作者:
赵天生,E-mail:zhaots@nxu.edu.cn;张建利,E-mail:zhangjl@nxu.edu.cn;Fax:0951-2062323。