Fe<sub>3</sub>O<sub>4</sub>纳米催化剂的制备及其F-T合成性能研究

涂军令; 徐勇军; 定明月; 王铁军; 马隆龙; 王敏龙

Fe₃O₄纳米催化剂的制备及其F-T合成性能研究

1.
中国科学院广州能源研究所, 广东广州 510640;
2.
东莞理工学院能源与化工系, 广东东莞 523808;
3.
中国科学院山西煤炭化学研究所, 山西太原 030001

基金项目: 国家自然科学基金(U1362109, 51206172); 国家重点基础研究发展规划(973 计划, 2013CB228105); 广东省科技计划项目(2013B010405012); 中国科学院战略性先导科技专项课题(XDA05010108)。

详细信息

通讯作者:
定明月

中图分类号: O643
计量
- 文章访问数: 437
- HTML全文浏览量: 20
- PDF下载量: 364
- 被引次数: 0
出版历程
- 收稿日期: 2015-05-04
- 修回日期: 2015-06-27
- 刊出日期: 2015-07-30

Preparation of nano-structured Fe₃O₄ catalysts and their performance in Fischer-Tropsch synthesis

1.
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China;
2.
Department of Energy and Chemical Engineering, Dongguan University of Technology, Dongguan 523808, China;
3.
Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China

摘要

摘要: 基于溶剂热合成体系,制备了不同形貌的Fe₃O₄微球和纳米片催化剂,考察了水热合成条件对Fe₃O₄晶粒形貌的影响,并研究了Fe₃O₄纳米催化剂的费托合成(F-T)性能。结果表明,成核和晶体生长速率是控制Fe₃O₄晶体形貌的关键。与传统的沉淀铁催化剂相比,Fe₃O₄纳米催化剂更容易还原和向活性相转变,因此,具有更高的F-T反应活性、低碳烯烃选择性及C₅₊选择性;Fe₃O₄微球催化剂比纳米片催化剂更易维晶粒的稳定,具有更高的反应活性和稳定性。
- Fe₃O₄纳米催化剂 /
- 晶体形貌 /
- 费托合成
Abstract: Two shape-defined nano-structured Fe₃O₄ catalysts such as Nano-Microsphere (FNM) and Nano-Flake (FNF) were prepared by a simple solvothermal method. The effects of precursor type on Fe₃O₄ crystal morphology was studied. It is found that the rate of nucleation and crystal growth have a crucial influence on the particle morphology. Compared to the traditional Fe catalyst, the shape-defined nano Fe₃O₄ catalysts could be easily reduced and transferred into active phases, resulting in higher Fischer-Tropsch synthesis (F-T) activity and C₅₊ selectivity. Especially, the FNM catalyst displayed higher catalytic activity and stability than the FNF catalyst. It was found that the FNF catalyst was more favorable to agglomeration because of shape change of the flakes. In addition, the results indicate that the hydrocarbon selectivity is strongly affected by the particle morphology.
- Fe₃O₄ nanocatalyst /
- morphology-defined nanoparticle /
- Fischer-Tropsch synthesis

HTML全文

参考文献(28)

DRY M E. The Fischer-Tropsch process: 1950-2000[J]. Catal Today, 2002, 71(3/4): 227-241.

LIU Z P, HU P. A new insight into Fischer-Tropsch synthesis[J]. J Am Chem Soc, 2002, 124(39): 11568-11569.

JAHANGIRI H, BENNETT J, MAHJOUBI P, WILSON K, GU S. A review of advanced catalyst development for Fischer-Tropsch synthesis of hydrocarbons from biomass derived syn-gas[J]. Catal Sci Technol, 2014, 4(8): 2210-2229.

STEYNBERG A, DRY M. Fischer-Tropsch technology[M]. Elsevier, Amsterdam, 2004.

DAVIS B H, OCCELLI M L. Fischer-Tropsch synthesis, catalysts and catalysis[M]. Elsevier, Amsterdam, 2006.

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

BELL A T. The impact of nanoscience on heterogeneous catalysis[J]. Science, 2003, 299(5613): 1688-1691.

MURZIN D Y. Size-dependent heterogeneous catalytic kinetics[J]. J Mol Catal A: Chem, 2010, 315(2): 226-230.

SHROFF M D, KALAKKAD D S, COULTER K E, KOHLER S D, HARRINGTON M S, JACKSON N B, SAULT A G, DATYE A K. Activation of precipitated iron Fischer-Tropsch synthesis catalysts[J]. J Catal, 1995, 156(2): 185-207.

OBRIEN R J, XU L G, SPICER R L, DAVIS B H. Activation study of precipitated iron Fischer-Tropsch catalysts[J]. Energy Fuel, 1996, 10(4): 921-926.

RIEDEL T, SCHULZ H, SCHAUB G, JUN K W, HWANG J S, LEE K W. Fischer-Tropsch on iron with H₂/CO and H₂/CO₂ as synthesis gases: The episodes of formation of the Fischer-Tropsch regime and construction of the catalyst[J]. Top Catal, 2003, 26(1/4): 41-54.

BRATLIE K M, LEE H, KOMVOPOULOS K, YANG P D, SOMORJAI G A. Platinum nanoparticle shape effects on benzene hydrogenation selectivity[J]. Nano Lett, 2007, 7(10): 3097-3101.

YANG C, ZHAO H B, HOU Y L, MA D. Fe5C2 nanoparticles: A facile bromide-induced synthesis and as an active phase for Fischer-Tropsch synthesis[J]. J Am Chem Soc, 2012, 134(38): 15814-15821.

CALDERONE V R, SHIJU N R, CURULLA-FERRE D, CHAMBREY S, KHODAKOV A, ROSE A, THIESSEN J, JESS A, ROTHENBERG G. De novo design of nanostructured iron-cobalt Fischer-Tropsch catalysts [J]. Angew Chem Int Edit, 2013, 52(16): 4397-4401.

PATZKE G R, ZHOU Y, KONTIC R, CONRAD F. Oxide nanomaterials: Synthetic developments, mechanistic studies, and technological innovations[J]. Angew Chem Int Edit, 2011, 50(4): 826-859.

POLARZ S. Shape matters: Anisotropy of the morphology of inorganic colloidal particles-synthesis and function[J]. Adv Funct Mater, 2011, 21(17): 3214-3230.

CHEN M, WU B H, YANG J, ZHENG N F. Small adsorbate-assisted shape control of Pd and Pt nanocrystals[J]. Adv Mat, 2012, 24(7): 862-879.

SCHMIDT E, VARGAS A, MALLAT T, BAIKER A. Shape-selective enantioselective hydrogenation on Pt nanoparticles[J]. J Am Chem Soc, 2009, 131(34): 12358-12367.

VAN BOKHOVEN J A. Understanding structure-performance relationships in oxidic catalysts: Controlling shape and tuning performance[J]. ChemCatChem, 2009, 1(3): 363-364.

XIE X W, SHEN W J. Morphology control of cobalt oxide nanocrystals for promoting their catalytic performance[J]. Nanoscale, 2009, 1(1): 50-60.

ZHOU K B, LI Y D. Catalysis based on nanocrystals with well-defined Facets[J]. Angew Chem Int Edit, 2012, 51(3): 602-613.

BUKUR D B, MUKESH D, PATEL S A. Promoter effects on precipitated iron catalysts for Fischer-Tropsch synthesis[J]. Ind Eng Chem Res, 1990, 29(2): 194-204.

LAMER V K. Nucleation in phase transitions[J]. Ind Eng Chem, 1952, 44(6): 1270-1277.

LUO M S, O'BRIEN R, DAVIS B H. Effect of palladium on iron Fischer-Tropsch synthesis catalysts[J]. Catal Lett, 2004, 98(1): 17-22.

KANG S H, BAE J W, PRASAD P S S, JUN K W. Fischer-Tropsch synthesis using zeolite-supported iron catalysts for the production of light hydrocarbons[J]. Catal Lett, 2008, 125(3/4): 264-270.

DAVIS B H. Fischer-Tropsch synthesis: Reaction mechanisms for iron catalysts[J]. Catal Today, 2009, 141(1-2): 25-33.

HERRANZ T, ROJAS S, PEREZ-ALONSO F J, OJEDA M, TERREROS P, FIERRO J L G. Genesis of iron carbides and their role in the synthesis of hydrocarbons from synthesis gas[J]. J Catal, 2006, 243(1): 199-211.

GALVIS H M T, BITTER J H, DAVIDIAN T, RUITENBEEK M, DUGULAN A I, DE JONG K P. Iron particle size effects for direct production of lower olefins from synthesis gas[J]. J Am Chem Soc, 2012, 134(39): 16207-16215.

施引文献

资源附件(0)

访问统计