Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance

LI Zhi-wen; CHEN Cong-biao; WANG Jun-gang; LIN Ming-gui; HOU Bo; JIA Li-tao; LI De-bao

Volume 47 Issue 6

Jun. 2019

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LI Zhi-wen, CHEN Cong-biao, WANG Jun-gang, LIN Ming-gui, HOU Bo, JIA Li-tao, LI De-bao. Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance[J]. Journal of Fuel Chemistry and Technology, 2019, 47(6): 709-717.

Citation:

LI Zhi-wen, CHEN Cong-biao, WANG Jun-gang, LIN Ming-gui, HOU Bo, JIA Li-tao, LI De-bao. Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance[J]. Journal of Fuel Chemistry and Technology, 2019, 47(6): 709-717.

Citation:

LI Zhi-wen, CHEN Cong-biao, WANG Jun-gang, LIN Ming-gui, HOU Bo, JIA Li-tao, LI De-bao. Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance[J]. Journal of Fuel Chemistry and Technology, 2019, 47(6): 709-717.

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Nitrogen-doped mesoporous carbon supported FeCu bimetallic catalyst and its CO hydrogenation performance

LI Zhi-wen^{1, 2},
CHEN Cong-biao^1
,,
WANG Jun-gang¹,
LIN Ming-gui¹,
HOU Bo¹,
JIA Li-tao^{1, 3
,},
LI De-bao^{1, 3}

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
3.
Dalian National Laboratory for Clean Energy, Dalian 116023, China

Funds:

Basic Applied Research Project of Shanxi 201601D021044

Strategic Priority Research Program of the Chinese Academy of Sciences XDA21020202

More Information

Corresponding author: CHEN Cong-biao, Tel: +86-0351-4040428, E-mail: congbiao_chen@sxicc.ac.cn; JIA Li-tao, Tel:+86-0351-4121877E-mail:Jialitao910@163.com
Received Date: 2019-01-26
Rev Recd Date: 2019-03-19

Available Online: 2021-01-23

Publish Date: 2019-06-10

Abstract

Abstract

In this work, nitrogen-doped mesoporous carbon (NDMC) was prepared by a hard template method, and the NDMC supported FeCu bimetallic catalysts were prepared by an impregnation method. The physical and chemical properties and CO hydrogenation performance of the catalysts with varying Fe/Cu ratios were studied. The results indicated that Cu-N had strong interaction which directly promoted Cu dispersion on the support. At a relatively high metal loading (45.0%-50.0%), Cu maintained uniform distribution similar to that of N, and the ratios of Fe/Cu on the catalyst surface were smaller than those in the bulk phase, which were different from precipitated Fe-Cu bimetallic catalysts. The XPS results showed that Cu was an electron donor, and the electrons in the Cu-N shifted to Fe. Compared with Fe/NDMC, the reduction of Fe_xCu_y/NDMC was facilitated, and their CO hydrogenation activity was significantly increased. Under the pretreatment conditions (H₂, 300℃), Fe was not completely reduced, and H might mainly interact with Fe-O in the form of Fe-O-H, while Cu-N interaction was stronger than Cu-H, resulting in a decrease in the ratio of surface active carbon/hydrogen, leading to a gradual increase in C₅₊ selectivity with the decrease of Fe/Cu ratio. Meanwhile, the introduction of Cu inhibited CO dissociation to some extent, and the electron migration ability of the support to the metal gradually increased with decreasing Fe/Cu ratio, and as a result the surface alkalinity of the catalysts increased with increasing Cu content, leading to further enhancement of C₅₊ selectivity and alcohol selectivity.
- nitrogen-doped mesoporous carbon,
- FeCu bimetal,
- interaction,
- CO hydrogenation

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References(35)

References

[1]	LIAND C D, LI Z J, DAI S. Mesoporous carbon materials:synthesis and modification[J]. Angew Chem Int Ed Eng, 2008, 47(20):3696-3717. doi: 10.1002/(ISSN)1521-3773
[2]	FU T J, LI Z H. Review of recent development in Co-based catalysts supported on carbon materials for Fischer-Tropsch synthesis[J]. Chem Eng Sci, 2015, 135:3-20. doi: 10.1016/j.ces.2015.03.007
[3]	XIONG H F, JEWELL L L, COVILLE N J. Shaped carbons as supports for the catalytic conversion of syngas to clean fuels[J]. ACS Catal, 2015, 5(4):2640-2658. doi: 10.1021/acscatal.5b00090
[4]	刘云朋, 周洁, 李中坚, 雷乐成.氮掺杂有序介孔碳的研究进展[J].现代化工, 2014, 34(6):19-22. http://d.old.wanfangdata.com.cn/Periodical/xdhg201406006 LIU Yun-peng, ZHOU Jie, LI Zhong-jian, LEI Le-cheng. Research progress of N-doped ordered mesoporous carbon[J]. Mod Chem Ind, 2014, 34(6):19-22. http://d.old.wanfangdata.com.cn/Periodical/xdhg201406006
[5]	李烁, 姚楠.掺氮碳基材料在费托合成反应中的应用[J].化工进展, 2015, 34(11):3933-3937. http://d.old.wanfangdata.com.cn/Periodical/hgjz201511020 LI Suo, YAO Nan. Application of nitrogen-doped carbon materials in Fischer-Tropsch synthesis reaction[J]. Chem Ind Eng Prog, 2015, 34(11):3933-3937. http://d.old.wanfangdata.com.cn/Periodical/hgjz201511020
[6]	SANKAR M, DIMITRATOS N, MIEDZIAK P J, WELLS P P, KIELY C J, HUTCHING G J. Designing bimetallic catalysts for a green and sustainable future[J]. Chem Soc Rev, 2012, 41(24):8099-8139. doi: 10.1039/c2cs35296f
[7]	WANG G H, CAO Z W, GU D, PFANDER N, SWERTZ A C, SPLIETHOFF B, BONGARD H J, WEIDENTHALER C, SCHMIDT W, RINALDI R, SCHUTH F. Nitrogen-doped ordered mesoporous carbon supported bimetallic PtCo nanoparticles for upgrading of biophenolics[J]. Angew Chem Int Ed, 2016, 55(31):8850-8855. doi: 10.1002/anie.201511558
[8]	XIAO K, QI X Z, BAO Z H, WANG X X, ZHONG L S, FANG K G, LIN M G, SUN Y H. CuFe, CuCo and CuNi nanoparticles as catalysts for higher alcohol synthesis from syngas:A comparative study[J]. Catal Sci Technol, 2013, 3(6):1591-1602. doi: 10.1039/c3cy00063j
[9]	XIAO K, BAO Z H, QI X Z, WANG X X, ZHONG L S, LIN M G, FANG K G. Unsupported CuFe bimetallic nanoparticles for higher alcohol synthesis via syngas[J]. Catal Commun, 2013, 40:154-157. doi: 10.1016/j.catcom.2013.06.024
[10]	KHODAKOV A Y, CHU W, FONGARLAND P. Advances in the development of novel cobalt Fischer-Tropsch catalysts for synthesis of long-chain hydrocarbons and clean fuels[J]. Chem Rev, 2007, 107(5):1692-1744. doi: 10.1021/cr050972v
[11]	LI S Z, LI A W, KRISHNAMOORTHY S, IGLESIA E. Effects of Zn, Cu, and K promoters on the structure and on the reduction, carburization, and catalytic behavior of iron-based Fischer-Tropsch synthesis catalysts[J]. Catal Lett, 2001, 77(4):197-205. doi: 10.1023/A:1013284217689
[12]	GAO W, ZHAO Y F, LIU J M, HUANG Q W, HE S, LI C M, ZHAO J W, WEI M. Catalytic conversion of syngas to mixed alcohols over CuFe-based catalysts derived from layered double hydroxides[J]. Catal Sci Technol, 2013, 3(5):1324-1332. doi: 10.1039/c3cy00025g
[13]	XIAO K, BAO Z H, QI X Z, WANG X X, ZHONG L S, FANG K G, LIN M G, SUN Y H. Structural evolution of CuFe bimetallic nanoparticles for higher alcohol synthesis[J]. J Mol Catal A:Chem, 2013, 378(11):319-325. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=4dd29ff2a1b453d66d1921ffbf802631
[14]	SHI X P, YU H B, GAO S, LI X Y, FANG H H, LI R J, LI Y Y, ZHANG L J, LIANG X L, YUAN Y Z. Synergistic effect of nitrogen-doped carbon-nanotube-supported Cu-Fe catalyst for the synthesis of higher alcohols from syngas[J]. Fuel, 2017, 210:241-248. doi: 10.1016/j.fuel.2017.08.064
[15]	KIATPHUENGPORN S, CHAREONPANICH M, LIMTRAKUL J. Effect of unimodal and bimodal MCM-41 mesoporous silica supports on activity of Fe-Cu catalysts for CO₂ hydrogenation[J]. Chem Eng J, 2014, 240:527-533. doi: 10.1016/j.cej.2013.10.090
[16]	WANG S, ZHAO Q, WEI H, WANG J Q, CHO M, CHO H S, TERASAKI O, WAN Y. Aggregation-free gold nanoparticles in ordered mesoporous carbons:Toward highly active and stable heterogeneous catalysts[J]. J Am Chem Soc, 2013, 135(32):11849-11860. doi: 10.1021/ja403822d
[17]	LIU G G, CHEN Q J, OYUNKHAND E, DING S Y, YAMANE N, YANG G H, YONEYAMA Y, TSUBAKI N. Nitrogen-rich mesoporous carbon supported iron catalyst with superior activity for Fischer-Tropsch synthesis[J]. Carbon, 2018, 130:304-314. doi: 10.1016/j.carbon.2018.01.015
[18]	XIONG H F, MOYO M, RAYNER M, JEWELL L L, BILLING D G, COVILLE N. Autoreduction and catalytic performance of a cobalt Fischer-Tropsch synthesis catalyst supported on nitrogen-doped carbon spheres[J]. ChemCatChem, 2010, 2(5):514-518. doi: 10.1002/cctc.200900309
[19]	DING Y Q, YANG J H, YANG G Z, LI P. Fabrication of ordered mesoporous carbons anchored with MnO nanoparticles through dual-templating approach for supercapacitors[J]. Ceram Int, 2015, 41(8):9980-9987. doi: 10.1016/j.ceramint.2015.04.078
[20]	LU J Z, YANG L J, XU B L, WU Q, ZHANG D, YUAN S J, ZHAI Y P, WANG X Z, FAN Y N, HU Z. Promotion effects of nitrogen doping into carbon nanotubes on supported iron Fischer-Tropsch catalysts for lower olefins[J]. ACS Catal, 2014, 4(2):613-621. doi: 10.1021/cs400931z
[21]	CHE R C, LIANG C Y, SHI H L, ZHOU X G, YANG X N. Electron energy-loss spectroscopy characterization and microwave absorption of iron-filled carbon-nitrogen nanotubes[J]. Nanotechnol, 2007, 18(35):355705. doi: 10.1088/0957-4484/18/35/355705
[22]	KIM S J, PARK Y J, RA E J, KIM K K, AN K H, LEE Y H, CHOI J Y, PARK C H, DOO S G, PARK M H, YANG C W. Defect-induced loading of Pt nanoparticles on carbon nanotubes[J]. Appl Phy Lett, 2007, 90(2):169. http://cn.bing.com/academic/profile?id=d27ae3c591d5f6db681c7e7d91661e15&encoded=0&v=paper_preview&mkt=zh-cn
[23]	BARTOLOME L, IMRAN M, LEE K G, SANGALANG A, AHN J K, KIM D H. Superparamagnetic γ-Fe₂O₃ nanoparticles as an easily recoverable catalyst for the chemical recycling of PET[J]. Green Chem, 2014, 16(1):279-286. doi: 10.1039/C3GC41834K
[24]	LI F, ZHANG L H, EVANS D G, DUAN X. Structure and surface chemistry of manganese-doped copper-based mixed metal oxides derived from layered double hydroxides[J]. Colloids Surfaces A, 2004, 244(1):169-177. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=7ee0110808fbd57b633b0f8aa7605439
[25]	LUK H T, MONDELLI C, MITCHELL S, SIOL S, STEWART J A, FERRE D C, PEREZ-RAMIREZ J. Role of carbonaceous supports and potassium promoter on higher alcohols synthesis over copper-iron catalysts[J]. ACS Catal, 2018, 8(10):9604-9618. doi: 10.1021/acscatal.8b02714
[26]	SUN F G, LIU J, CHEN H C, ZHANG Z X, QIAO W M, LONG D H, LING L C. Nitrogen-rich mesoporous carbons:Highly efficient, regenerable metal-free catalysts for low-temperature oxidation of H₂S[J]. ACS Catal, 2013, 3(5):862-870. doi: 10.1021/cs300791j
[27]	BAGUS P S, ILTON E, NELIN C J. The interpretation of XPS spectra:Insights into materials properties[J]. Surf Sci Rep, 2013, 68(2):273-304. doi: 10.1016/j.surfrep.2013.03.001
[28]	YANG X M, WEI Y, SU Y L, ZHOU L P. Characterization of fused Fe-Cu based catalyst for higher alcohols synthesis and DRIFTS investigation of TPSR[J]. Fuel Process Technol, 2010, 91(9):1168-1173. doi: 10.1016/j.fuproc.2010.03.032
[29]	ZHANG C H, ZHAO G Y, LIU K K, YANG Y, XIANG H W, LI Y W. Adsorption and reaction of CO and hydrogen on iron-based Fischer-Tropsch synthesis catalysts[J]. J Mol Catal A:Chem, 2010, 328(1/2):35-43. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=ffab8b7babce08c8ff4afb536239815a
[30]	BLIEM R, VAN DER HOEVEN J, ZAVODNY A, GAMBA O, PAVELEC J, DE JONGH P E, SCHMID M, DIEBOLD U, PARKINSON G S. An atomic-scale view of CO and H₂ oxidation on a Pt/Fe₃O₄model catalyst[J]. Angew Chem Int Ed, 2015, 127(47):14205-14208. doi: 10.1002/ange.201507368
[31]	AL-DOSSARY M, FIERRO J L G, SPIVEY J J. Cu-promoted Fe₂O₃/MgO-based Fischer-Tropsch catalysts of biomass-derived syngas[J]. Ind Eng Chem Res, 2015, 54(3):911-921. doi: 10.1021/ie504473a
[32]	MAO W Y, MA H F, ZHANG H T, SUN Q W, YING W Y. Influence of copper loading on the surface species and catalytic properties in the formation of oxygenated by-products during FTS over FeCuKLa/SiO₂catalysts[J]. Catal Lett, 2012, 142(9):1098-1106. doi: 10.1007/s10562-012-0865-6
[33]	KANG S H, KOO H M, KIM A R, LEE D H, RYU J H, YOO Y D, BAE J W. Correlation of the amount of carbonaceous species with catalytic performance on iron-based Fischer-Tropsch catalysts[J]. Fuel Process Technol, 2013, 109:141-149. doi: 10.1016/j.fuproc.2012.09.052
[34]	ZHANG C H, YANG Y, TENG B T, LI T Z, ZHENG H Y, XIANG H W, LI Y W. Study of an iron-manganese Fischer-Tropsch synthesis catalyst promoted with copper[J]. J Catal, 2006, 237(2):405-415. http://cn.bing.com/academic/profile?id=c65080a18786083e192f4d736240d190&encoded=0&v=paper_preview&mkt=zh-cn
[35]	CHONCO Z H, LODYA L, CLAEYS M, STEEN E V. Copper ferrites:A model for investigating the role of copper in the dynamic iron-based Fischer-Tropsch catalyst[J]. J Catal, 2013, 308:363-373. doi: 10.1016/j.jcat.2013.08.012