MoO<sub>3</sub>-SnO<sub>2</sub> catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation

YANG Qi; GAO Xiu-juan; FENG Ru; LI Ming-jie; ZHANG Jun-feng; ZHANG Qing-de; HAN Yi-zhuo; TAN Yi-sheng

Volume 47 Issue 8

Aug. 2019

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2019 > 47(8): 934-941

YANG Qi, GAO Xiu-juan, FENG Ru, LI Ming-jie, ZHANG Jun-feng, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. MoO3-SnO2 catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation[J]. Journal of Fuel Chemistry and Technology, 2019, 47(8): 934-941.

Citation:

YANG Qi, GAO Xiu-juan, FENG Ru, LI Ming-jie, ZHANG Jun-feng, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. MoO₃-SnO₂ catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation[J]. Journal of Fuel Chemistry and Technology, 2019, 47(8): 934-941.

Citation:

PDF( 6172 KB)

MoO₃-SnO₂ catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation

YANG Qi^{1, 2},
GAO Xiu-juan^{1, 2},
FENG Ru^{1, 2},
LI Ming-jie^{1, 2},
ZHANG Jun-feng¹,
ZHANG Qing-de^{1
,
,},
HAN Yi-zhuo¹,
TAN Yi-sheng¹

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 21773283

the National Natural Science Foundation of China 21373253

CAS Interdisciplinary Innovation Team BK2018001

Youth Innovation Promotion Association CAS 2014155

the Open Project Program of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University 201624

More Information

Corresponding author: ZHANG Qing-de, Tel: +86-351-4044388; Fax: +86-351-4044287, E-mail: qdzhang@sxicc.ac.cn
Received Date: 2019-03-26
Rev Recd Date: 2019-05-28

Available Online: 2021-01-23

Publish Date: 2019-08-10

Abstract

Abstract

MoO₃-SnO₂ composite metal oxide catalyst was synthesized by one-step hydrothermal synthesis method without precipitant. The effect of MoO_x dispersion state on the catalytic performance of MoO₃-SnO₂ catalysts with different Mo/Sn molar ratios was investigated for dimethyl ether (DME) low-temperature oxidation to methyl formate (MF). MF selectivity reaches 77.6% with DME conversation of 22.0% over Mo₁Sn₂ at 150 ℃. The physiochemical properties of these catalysts were characterized by TEM, XRD, Raman, FT-IR, NH₃-TPD and H₂-TPR. The results showed that the addition of SnO₂ into MoO₃ affected the crystal structure of catalysts, forming MoO_x species with different degree of dispersion on the surface of SnO₂. The special architecture of MoO_x-SnO₂ plays a major role in modifying the acidity and the oxidizability of MoO₃-SnO₂ catalysts, leading to the obvious differences on catalytic activity.
- hydrothermal synthesis,
- dimethyl ether,
- selective oxidation,
- methyl formate,
- MoO_x

FullText(HTML)

References(33)

References

[1]	SEMELSBERGER T A, BORUP R L, GREENE H L. Dimethyl ether(DME) as an alternative fuel[J]. J Power Sources, 2006, 156(2):497-511. doi: 10.1016/j.jpowsour.2005.05.082
[2]	XU M T, LUNSFORD J H, GOODMAN D W, BHATTACHARYYA A. Synthesis of dimethyl ether (DME) from methanol over solid-acid catalysts[J]. Appl Catal A:Gen, 1997, 149(2):289-301. doi: 10.1016/S0926-860X(96)00275-X
[3]	TAN Y S, XIE H J, CUI H T, HAN Y Z, ZHONG B. Modification of Cu-based methanol synthesis catalyst for dimethyl ether synthesis from syngas in slurry phase[J]. Catal Today, 2005, 104(1):25-29. http://cn.bing.com/academic/profile?id=a3050a170c64e3903ca6807b9414d6db&encoded=0&v=paper_preview&mkt=zh-cn
[4]	SUN J, YANG G H, YONEYAMA Y, TSUBAKI N. Catalysis chemistry of dimethyl ether synthesis[J]. ACS Catal, 2014, 4(10):3346-3356. doi: 10.1021/cs500967j
[5]	孙明, 余林, 孙长勇, 宋一兵, 孙建.二甲醚的应用及下游产品开发[J].精细化工, 2003, 20(11):695-699. doi: 10.3321/j.issn:1003-5214.2003.11.017 SUN Ming, YU Lin, SUN Chang-yong, SONG Yi-bing, SUN Jian. Application of Dimethyl ether and development of its downstream products[J]. Fine Chem, 2003, 20(11):695-699. doi: 10.3321/j.issn:1003-5214.2003.11.017
[6]	ZHANG Q D, TAN Y S, LIU G B, ZHANG J F, HAN Y Z. Rhenium oxide-modified H₃PW₁₂O₄₀/TiO₂ catalysts for selective oxidation of dimethyl ether to dimethoxy dimethyl ether[J]. Green Chem, 2014, 16(11):4708-4715. doi: 10.1039/C4GC01373E
[7]	ZHANG Q D, WANG W F, ZHANG Z Z, HAN Y Z, TAN Y S. Low-temperature oxidation of dimethyl ether to polyoxymethylene dimethyl ethers over CNT-supported rhenium catalyst[J]. Catalysts, 2016, 6(3):43. doi: 10.3390/catal6030043
[8]	GAO X J, WANG W F, GU Y Y, ZHANG Z Z, ZHANG J F, ZHANG Q D, TSUBAKI N, HAN Y Z, TAN Y S. Synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation over carbon-based catalysts[J]. ChemCatChem, 2018, 10(1):273-279. doi: 10.1002/cctc.v10.1
[9]	ZHANG Z Z, ZHANG Q D, JIA L Y, WANG W F, XIAO H, HAN Y Z, TSUBAKI N, TAN Y S. Effects of MoO₃ crystalline structure of MoO₃-SnO₂ catalysts on selective oxidation of glycol dimethyl ether to 1, 2-propandiol[J]. Catal Sci Technol, 2016, 6(6):1842-1849. doi: 10.1039/C5CY00894H
[10]	HUANG X M, LIU J L, CHEN J L, XU Y D, SHEN W J. Mechanistic study of selective oxidation of dimethyl ether to formaldehyde over alumina-supported molybdenum oxide catalyst[J]. Catal Lett, 2006, 108(1/2):79-86. http://cn.bing.com/academic/profile?id=7fd08a98c45253b3194327f57adaf6d4&encoded=0&v=paper_preview&mkt=zh-cn
[11]	高秀娟, 王文峰, 张振洲, 张清德, 谭猗生, 韩怡卓.二甲醚氧化制聚甲氧基二甲醚的研究进展[J].石油化工, 2017, 46(2):143-150. http://d.old.wanfangdata.com.cn/Periodical/syhg201702001 GAO Xiu-juan, WANG Wen-feng, ZHANG Zhen-zhou, ZHANG Qing-de, TAN Yi-sheng, HAN Yi-zhuo. Progresses in synthesis of polymethylene dimethyl ethers from dimethyl ether[J]. Petrochem Technol, 2017, 46(2):143-150. http://d.old.wanfangdata.com.cn/Periodical/syhg201702001
[12]	汪多仁.甲酸甲酯的生产发展与应用前景[J].石油与天然气化工, 1998, 27(3):149-151. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=QK199800540043 WANG Duo-ren. Production development and application prospects of methyl formate[J]. Chem Eng Oil Gas, 1998, 27(3):149-151. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=QK199800540043
[13]	周寿祖.甲酸甲酯的生产技术和应用前景[J].化工科技市场, 2003, 26(2):13-18. http://d.old.wanfangdata.com.cn/Periodical/hgkjsc200302004 ZHOU Shou-zu. Production technology and application foreground of methyl formate[J]. Chem Technol Market, 2003, 26(2):13-18. http://d.old.wanfangdata.com.cn/Periodical/hgkjsc200302004
[14]	AI M. The production of methyl formate by the vapor-phase oxidation of methanol[J]. J Catal, 1982, 77(1):279-288. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=e3f3f3492468b3d76c12c7ba1bdb1945
[15]	AI M. The reaction of formaldehyde on various metal-oxide catalysts[J]. J Catal, 1983, 83(1):141-150. doi: 10.1016-0021-9517(83)90037-4/
[16]	LIU H C, CHEUNG P, IGLESIA E. Structure and support effects on the selective oxidation of dimethyl ether to formaldehyde catalyzed by MoO_x domains[J]. J Catal, 2003, 217(1):222-232. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=180d6d3f82f0282854bdd2714ae015e2
[17]	LIU H C, CHEUNG P, IGLESIA E. Effects of Al₂O₃ support modifications on MoO_x and VO_x catalysts for dimethyl ether oxidation to formaldehyde[J]. Phys Chem Chem Phys, 2003, 5(17):3795-3800. doi: 10.1039/b302776g
[18]	LIU G B, ZHANG Q D, HAN Y Z, TSUBAKI N, TAN Y S. Selective oxidation of dimethyl ether to methyl formate over trifunctional MoO₃-SnO₂ catalyst under mild conditions[J]. Green Chem, 2013, 15(6):1501-1504. doi: 10.1039/c3gc40279g
[19]	LIU G B, ZHANG Q D, HAN Y Z, TSUBAKI N, TAN Y S. Effects of the MoO₃ structure of Mo-Sn catalysts on dimethyl ether oxidation to methyl formate under mild conditions[J]. Green Chem, 2015, 17(2):1057-1064. doi: 10.1039/C4GC01591F
[20]	刘广波, 张清德, 韩怡卓, 椿范立, 谭猗生. MoO₃-SnO₂催化剂上二甲醚低温氧化高选择性制备甲酸甲酯[J].燃料化学学报, 2013, 41(2):223-227. doi: 10.3969/j.issn.0253-2409.2013.02.015 LIU Guang-bo, ZHANG Qing-de, HAN Yi-zhuo, TSUBAKI Noritatsu, TAN Yi-sheng. Low-temperature oxidation of dimeyhyl ether to methyl formate with high selectivity over MoO₃-SnO₂ catalysts[J]. J Fuel Chem Technol, 2013, 41(2):223-227. doi: 10.3969/j.issn.0253-2409.2013.02.015
[21]	ZHANG Z Z, ZHANG Q D, JIA L Y, WANG W F, ZHANG T, HAN Y Z, TSUBAKI N, TAN Y S. Effects of tetrahedral molybdenum oxide species and MoO_x domains on the selective oxidation of dimethyl ether under mild conditions[J]. Catal Sci Technol, 2016, 6(9):2975-2983. doi: 10.1039/C5CY01569C
[22]	ZHANG Z, ZHANG Q, JIA L, WANG W, TIAN S P, WANG P, XIAO H, HAN Y, TSUBAKI N, TAN Y. The effects of the Mo-Sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature[J]. Catal Sci Technol, 2016, 6(15):6109-6117. doi: 10.1039/C6CY00460A
[23]	DEVAN R S, PATIL R A, LIN J H, MA Y R. One-dimensional metal-oxide nanostructures:Recent developments in synthesis, characterization, and applications[J]. Adv Funct Mater, 2012, 22(16):3326-3370. doi: 10.1002/adfm.v22.16
[24]	赵延霞.水热法合成一维纳米级MoO₃微粉[J].中国钨业, 2012, 27(3):25-29. doi: 10.3969/j.issn.1009-0622.2012.03.007 ZHAO Yan-xia. Synthesis the one-dimensional nano-size MoO₃ via acidification for hydrolyzing[J]. China Tungsten Ind, 2012, 27(3):25-29. doi: 10.3969/j.issn.1009-0622.2012.03.007
[25]	张建荣, 高濂.水热法合成纳米SnO₂粉体[J].无机材料学报, 2004, 19(5):1177-1180. doi: 10.3321/j.issn:1000-324X.2004.05.034 ZHANG Jian-rong, GAO Lian. Hydrothermal synthesis of tin oxide nanoparticles[J]. J Inorg Mater, 2004, 19(5):1177-1180. doi: 10.3321/j.issn:1000-324X.2004.05.034
[26]	GONCALVES F, MEDEIROS P R S, EON J G, APPEL L G. Active sites for ethanol oxidation over SnO₂-supported molybdenum oxides[J]. Appl Catal A:Gen, 2000, 193(1/2):195-202. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=3e9f3819bf721b2b4608bb2ff36b370f
[27]	ROUTRAY K, ZHOU W, KIELY C J, GRUNERT W, WACHS I E. Origin of the synergistic interaction between MoO₃ and iron molybdate for the selective oxidation of methanol to formaldehyde[J]. J Catal, 2010, 275(1):84-98. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=acb38cb74d8ce4f1f2a27a98da4faf25
[28]	HERRMANN J M, VILLAIN F, APPEL L G. Characterization of Mo-Sn-O system by means of Raman spectroscopy and electrical conductivity measurements[J]. Appl Catal A:Gen, 2003, 240(1/2):177-182. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=ce15e10e291573e3004eb47ed48b1907
[29]	LAKSHMI L J, ALYEA E C. ESR, FT-Raman spectroscopic and ethanol partial oxidation studies on MoO₃/SnO₂ catalysts made by metal oxide vapor synthesis[J]. Catal Lett, 1999, 59(1):73-77. https://www.onacademic.com/detail/journal_1000034816457110_b8a9.html
[30]	HABER J, LALIK E. Catalytic properties of MoO₃ revisited[J]. Catal Today, 1997, 33(1/3):119-137. https://www.sciencedirect.com/science/article/abs/pii/S0920586196001071
[31]	NIWA M, IGARASHI J. Role of the solid acidity on the MoO₃ loaded on SnO₂ in the methanol oxidation into formaldehyde[J]. Catal Today, 1999, 52(1):71-81. https://www.sciencedirect.com/science/article/abs/pii/S0920586199000644
[32]	FENG Q Y, YAO S L. Infrared study of ZrO₂ surface sites using adsorbed probe molecules. 2. Dimethyl ether adsorption[J]. J Phys Chem B, 2000, 104(47):11253-11257. doi: 10.1021/jp002509m
[33]	杜英辉, 许国基.氢气还原金属氧化物[J].原子能科学技术, 1999, 33(4):360-362. doi: 10.3969/j.issn.1000-6931.1999.04.020 DU Ying-hui, XU Guo-ji. Hydrogen reduction of metal oxides to metals[J]. Atom Energy Sci Technol, 1999, 33(4):360-362. doi: 10.3969/j.issn.1000-6931.1999.04.020