Citation: Pan XIONG, Xiu-juan GAO, Wen-xiu WANG, Jun-feng ZHANG, Fa-en SONG, Qing-de ZHANG, Yi-zhuo HAN, Yi-sheng TAN. Effect of calcination temperature on the structure and performance of molybdenum-tin catalyst for DME oxidation[J]. Journal of Fuel Chemistry and Technology, ;2022, 50(1): 63-71. doi: 10.1016/S1872-5813(21)60120-2 shu

Effect of calcination temperature on the structure and performance of molybdenum-tin catalyst for DME oxidation

Pan XIONG ^{1, 2} ,
Xiu-juan GAO ^{1, 2} ,
Wen-xiu WANG ^{1, 2} ,
Jun-feng ZHANG ¹ ,
Fa-en SONG ¹ ,
Qing-de ZHANG ^{1, 3,,} ,
Yi-zhuo HAN ¹ ,
Yi-sheng TAN ¹

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 10049, China
3.
Dalian National Laboratory for Clean Energy, Dalian 116023, China

Corresponding author: Qing-de ZHANG, qdzhang@sxicc.ac.cn
Received Date: 26 April 2021
Revised Date: 23 May 2021

Figures(10)

The Mo1Sn2 catalysts with a Mo/Sn molar ratio of 1∶2 were prepared by the hydrothermal method, and their structure was regulated by changing the calcination temperature (400–700 ℃). The effect of the structural transformation of catalysts on the performance of selective oxidation of dimethyl ether (DME) to methyl formate (MF) was studied. It was found that the Mo1Sn2 catalyst calcined at 400 ℃ exhibited good performance in the oxidation of DME to methyl formate, showing a DME conversion of 9.2% and the MF selectivity of 86.9% at 110 ℃ and under atmospheric pressure without the generation of CO_x. The catalysts were systematically characterized by XRD, Raman, XPS, TPD, H₂-TPR and in-situ FT-IR. The results showed that the low-temperature calcination was favorable for the formation of MoO_x structure and more Mo⁵⁺ species on the catalyst surface, resulting in the enhanced acidity and redox ability of the catalyst, and the increase of medium to strong basic sites on the catalysts. In such case, the activity and methyl formate production of the catalyst were significantly promoted.
- dimethyl ether oxidation,
- Mo1Sn2 catalyst,
- calcination temperature,
- structure,
- methyl formate
1. [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. [2]
  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
3. [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. doi: 10.1016/j.cattod.2005.03.033
4. [4]
  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
5. [5]
  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. [6]
  CHANG Yan-hong, HAN Yi-zhuo, WANG Xin-kui. Production, application and development of downstream products of dimethyl ether[J]. Nat Gas Chem Ind,2000,25(3):45−49.
7. [7]
  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.201701213
8. [8]
  ZHOU Shou-zu. Production technology and application foreground of methyl formate[J]. Chem Technol Market,2003,26(2):13−18.
9. [9]
  CHEN Wen-long, LIU Hai-chao. Catalysts and reaction pathways for dehydrogenation and selective oxidation methanol to methyl formate[J]. Chin Sci Bull,2015,60(16):1502−1512. doi: 10.1360/N972014-01349
10. [10]
  AI M. The production of methyl formate by the vapor-phase oxidation of methanol[J]. J Catal,1982,77(1):279−288. doi: 10.1016/0021-9517(82)90168-3
11. [11]
  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
12. [12]
  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
13. [13]
  CHEUNG P, LIU H C, IGLESIA E. Kinetics and mechanism of dimethyl ether oxidation to formaldehyde on supported molybdenum oxide domains[J]. J Phys Chem B,2004,108(48):18650−18658. doi: 10.1021/jp0477405
14. [14]
  LIU H C, CHEUNG P, IGLESIA E. Zirconia-supported MoO_x, catalysts for the selective oxidation of dimethyl ether to formaldehyde: Structure, redox properties, and reaction pathways[J]. J Phys Chem B,2003,107(17):4118−4127. doi: 10.1021/jp0221744
15. [15]
  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.
16. [16]
  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
17. [17]
  ZHANG Z Z, ZHANG Q D, JIA L Y, WANG W F, TIAN S P, WANG P, XIAO H, HAN Y Z, TSUBAKI N, TAN Y S. 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
18. [18]
  (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]. J Fuel Chem Technol,2019,47(8):934−941. doi: 10.3969/j.issn.0253-2409.2019.08.005
19. [19]
  LI A, LONG H, ZHANG H, LI H. High-yield synthesis of Ce modified Fe-Mn composite oxides benefitting from catalytic destruction of chlorobenzene[J]. Rsc Adv,2020,10(17):10030−10037. doi: 10.1039/C9RA10489E
20. [20]
  TAO Z, YANG Y, DING M, LI T, XIANG H, LI Y. Effect of calcination behaviors on precipitated iron-manganese Fischer-Tropsch synthesis catalyst[J]. Catal Lett,2007,117(3/4):130−135. doi: 10.1007/s10562-007-9118-5
21. [21]
  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
22. [22]
  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. doi: 10.1023/A:1019099900418
23. [23]
  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. doi: 10.1016/S0926-860X(02)00419-2
24. [24]
  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. doi: 10.1016/S0926-860X(99)00430-5
25. [25]
  HABER J, LALIK E. Catalytic properties of MoO₃ revisited[J]. Catal Today,1997,33(1/3):119−137. doi: 10.1016/S0920-5861(96)00107-1
26. [26]
  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
27. [27]
  TAO Dong-ping, YANG Xian-wan. Kinetics of disproportionation and reduction of stannous oxide and mechanism of reduction of stannic oxide[J]. Chin J Nonferrous Met,1998,8(1):126−130. doi: 10.3321/j.issn:1004-0609.1998.01.027
28. [28]
  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
29. [29]
  TAN X J, WANG L Z, CHENG C, YAN X F, SHEN B, ZHANG J L. Plasmonic MoO_3−x @MoO₃ nanosheets for highly sensitive SERS detection through nanoshell-isolated electromagnetic enhancement[J]. Chem Commun,2016,52(14):2893−2896. doi: 10.1039/C5CC10020H
30. [30]
  SWIATOWSKA-MROWIECKA J, DE DIESBACH S, MAURICE V, ZANNA S, KLEIN L, BRIAND E, VICKRIDGE I, MARCUS P. Li-ion intercalation in thermal oxide thin films of MoO₃ as studied by XPS, RBS, and NRA[J]. J Phys Chem C,2008,112(29):11050−11058. doi: 10.1021/jp800147f
31. [31]
  YANG Qi. Study on the mechanism of the low-temperature oxidation of dimethyl ether over MoO₃-SnO₂ catalyst[D]. Beijing: University of Chinese Academy of Sciences, 2019.
32. [32]
  LOCHAR V. FT-IR study of methanol, formaldehyde and methyl formate adsorption on the surface of Mo/Sn oxide catalyst[J]. Appl Catal A: Gen,2006,309(1):33−36. doi: 10.1016/j.apcata.2006.04.030
1. [1]
  Peng ZHOU , Xiao CAI , Qingxiang MA , Xu LIU . Effects of Cu doping on the structure and optical properties of Au₁₁(dppf)₄Cl₂ nanocluster. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1254-1260. doi: 10.11862/CJIC.20240047
2. [2]
  Xiao SANG , Qi LIU , Jianping LANG . Synthesis, structure, and fluorescence properties of Zn(Ⅱ) coordination polymers containing tetra-alkenylpyridine ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2124-2132. doi: 10.11862/CJIC.20240158
3. [3]
  Qin ZHU , Jiao MA , Zhihui QIAN , Yuxu LUO , Yujiao GUO , Mingwu XIANG , Xiaofang LIU , Ping NING , Junming GUO . Morphological evolution and electrochemical properties of cathode material LiAl_0.08Mn_1.92O₄ single crystal particles. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1549-1562. doi: 10.11862/CJIC.20240022
4. [4]
  Qiuyu Ming , Huijun Jiang , Zhihao Zhang . A Sightseeing Tour of Folic Acid Processing Plant. University Chemistry, 2024, 39(9): 11-15. doi: 10.12461/PKU.DXHX202404092
5. [5]
  Zhiwen HUANG , Qi LIU , Jianping LANG . W/Cu/S cluster-based supramolecular macrocycles and their third-order nonlinear optical responses. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 79-87. doi: 10.11862/CJIC.20240184
6. [6]
  Liuyun Chen , Wenju Wang , Tairong Lu , Xuan Luo , Xinling Xie , Kelin Huang , Shanli Qin , Tongming Su , Zuzeng Qin , Hongbing Ji . Soft template-induced deep pore structure of Cu/Al₂O₃ for promoting plasma-catalyzed CO₂ hydrogenation to DME. Acta Physico-Chimica Sinica, 2025, 41(6): 100054-0. doi: 10.1016/j.actphy.2025.100054
7. [7]
  Lifang HE , Wenjie TANG , Yaoze LUO , Mingsheng LIANG , Jianxin TANG , Yuxuan WU , Fuxing ZHANG , Xiaoming ZHU . Synthesis, structure, and anticancer activity of two dialkyltin complexes constructed based on 2, 2′-bipyridin-6, 6′-dicarboxylic acid. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1601-1609. doi: 10.11862/CJIC.20250012
8. [8]
  Qing Li , Guangxun Zhang , Yuxia Xu , Yangyang Sun , Huan Pang . P-Regulated Hierarchical Structure Ni₂P Assemblies toward Efficient Electrochemical Urea Oxidation. Acta Physico-Chimica Sinica, 2024, 40(9): 2308045-0. doi: 10.3866/PKU.WHXB202308045
9. [9]
  Yanhui Guo , Li Wei , Zhonglin Wen , Chaorong Qi , Huanfeng Jiang . Recent Progress on Conversion of Carbon Dioxide into Carbamates. Acta Physico-Chimica Sinica, 2024, 40(4): 2307004-0. doi: 10.3866/PKU.WHXB202307004
10. [10]
  Fangxuan Liu , Ziyan Liu , Guowei Zhou , Tingting Gao , Wenyu Liu , Bin Sun . 中空结构光催化剂. Acta Physico-Chimica Sinica, 2025, 41(7): 100071-0. doi: 10.1016/j.actphy.2025.100071
11. [11]
  Jianding LI , Junyang FENG , Huimin REN , Gang LI . Proton conductive properties of a Hf(Ⅳ)-based metal-organic framework built by 2,5-dibromophenyl-4,6-dicarboxylic acid. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1094-1100. doi: 10.11862/CJIC.20240464
12. [12]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
13. [13]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
14. [14]
  Wanting CHEN , Chufei MIAO , Yan LIU , Bobi ZHENG , Xiaoyu ZHENG , Han XU , Jumei TIAN . Syntheses, characterization, and luminescence properties of Yb(Ⅲ)-based one-dimensional chain coordination polymer. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1672-1680. doi: 10.11862/CJIC.20250013
15. [15]
  Hexing SONG , Zan SUN . Synthesis, crystal structure, Hirshfeld surface analysis, and fluorescent sensing for Fe³⁺ of an Mn(Ⅱ) complex based on 1-naphthalic acid. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 885-892. doi: 10.11862/CJIC.20240402
16. [16]
  Asif Hassan Raza , Shumail Farhan , Zhixian Yu , Yan Wu . Double S-Scheme ZnS/ZnO/CdS Heterostructure Photocatalyst for Efficient Hydrogen Production. Acta Physico-Chimica Sinica, 2024, 40(11): 2406020-0. doi: 10.3866/PKU.WHXB202406020
17. [17]
  Yahui HAN , Jinjin ZHAO , Ning REN , Jianjun ZHANG . Synthesis, crystal structure, thermal decomposition mechanism, and fluorescence properties of benzoic acid and 4-hydroxy-2, 2′: 6′, 2″-terpyridine lanthanide complexes. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 969-982. doi: 10.11862/CJIC.20240395
18. [18]
  Bing LIU , Huang ZHANG , Hongliang HAN , Changwen HU , Yinglei ZHANG . Visible light degradation of methylene blue from water by triangle Au@TiO₂ mesoporous catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 941-952. doi: 10.11862/CJIC.20230398
19. [19]
  Jingzhao Cheng , Shiyu Gao , Bei Cheng , Kai Yang , Wang Wang , Shaowen Cao . Construction of 4-Amino-1H-imidazole-5-carbonitrile Modified Carbon Nitride-Based Donor-Acceptor Photocatalyst for Efficient Photocatalytic Hydrogen Evolution. Acta Physico-Chimica Sinica, 2024, 40(11): 2406026-0. doi: 10.3866/PKU.WHXB202406026
20. [20]
  Yajin Li , Huimin Liu , Lan Ma , Jiaxiong Liu , Dehua He . Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO₂ over Au/Co₃O₄-ZnO Catalyst. Acta Physico-Chimica Sinica, 2024, 40(9): 2308005-0. doi: 10.3866/PKU.WHXB202308005

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(902)
HTML views(185)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142