Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst

WANG Wen-xiu; GAO Xiu-juan; XIONG Pan; ZHANG Jun-feng; SONG Fa-en; ZHANG Qing-de; HAN Yi-zhuo; TAN Yi-sheng

doi:10.1016/S1872-5813(21)60094-4

Volume 49 Issue 10

Oct. 2021

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Article Navigation > Journal of Fuel Chemistry and Technology > 2021 > 49(10): 1487-1494

WANG Wen-xiu, GAO Xiu-juan, XIONG Pan, ZHANG Jun-feng, SONG Fa-en, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst[J]. Journal of Fuel Chemistry and Technology, 2021, 49(10): 1487-1494. doi: 10.1016/S1872-5813(21)60094-4

Citation:

WANG Wen-xiu, GAO Xiu-juan, XIONG Pan, ZHANG Jun-feng, SONG Fa-en, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst[J]. Journal of Fuel Chemistry and Technology, 2021, 49(10): 1487-1494. doi: 10.1016/S1872-5813(21)60094-4

Citation:

WANG Wen-xiu, GAO Xiu-juan, XIONG Pan, ZHANG Jun-feng, SONG Fa-en, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst[J]. Journal of Fuel Chemistry and Technology, 2021, 49(10): 1487-1494. doi: 10.1016/S1872-5813(21)60094-4

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Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst

doi: 10.1016/S1872-5813(21)60094-4

WANG Wen-xiu^{1, 2
,},
GAO Xiu-juan^{1, 2},
XIONG Pan^{1, 2},
ZHANG Jun-feng¹,
SONG Fa-en¹,
ZHANG Qing-de^{1, 3
,
,},
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 10049, China
3.
Dalian National Laboratory for Clean Energy, Dalian 116023, China

Funds: The project was supported by the National Natural Science Foundation of China (21773283, 21373253), CAS Interdisciplinary Innovation Team (BK2018001), the Dalian National Laboratory For Clean Energy (DNL) Cooperation Fund, CAS (DNL 201903), the Youth Innovation Promotion Association CAS (2014155) and the Open Project Program of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University (201624)

Received Date: 2021-03-31
Rev Recd Date: 2021-04-21

Available Online: 2021-05-12

Publish Date: 2021-10-30

Abstract

Abstract

A new Mo-Sn catalyst prepared by hydrothermal method was used for the synthesis of dimethoxymethane (DMM) from methanol oxidation. The catalyst with low Mo content can achieve low-temperature oxidation of methanol to DMM with high selectivity. The influence of Mo content on the structure and the catalytic performance of the catalyst was investigated. It was found that Mo1Sn10 catalyst showed the best catalytic performance under the conditions of 140 °C and atmospheric pressure, the methanol conversion was 14.2%, and the selectivity of DMM reached 88.9% without the formation of CO_x during the reaction process. The catalysts were characterized by XRD, Raman, FT-IR, XPS, NH₃-TPD and H₂-TPR. The results showed that the catalysts with different Mo content had obvious differences in structure and performance. Lower Mo content was more conducive to the formation of Mo⁵⁺ and MoO_x, and the resulting changes in acidity and redox properties were the important reasons for the excellent performance of the catalysts.
- methanol,
- low temperature oxidation,
- dimethoxymethane,
- Mo-Sn catalyst,
- Mo⁵⁺species

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References(27)

References

[1]	LIU X M, LU G Q, YAN Z F, YAN Z F, JORGE B. Recent advances in catalysts for methanol synthesis via hydrogenation of CO and CO₂[J]. Ind Eng Chem Res,2003,42(25):6518−6530. doi: 10.1021/ie020979s
[2]	GRABOW L C, MAVRIKAKIS M. Mechanism of methanol synthesis on Cu through CO₂ and CO hydrogenation[J]. ACS Catal,2011,1(4):365−384. doi: 10.1021/cs200055d
[3]	BEHRENS M, STUDT F, KASATKIN I, KUHL S, HAVECKER M, ABILD-PEDERERSEN F, ZANDER S, GIRGSDIES F, KURR P, KNIEP B L, TOVAR M, FISCHER R W, NORSKOV J K, SCHLOGL R. The active site of methanol synthesis over Cu/ZnO/Al₂O₃ industrial catalysts[J]. Science,2012,336(3):893−897.
[4]	TIAN P, WEI Y, YE M, LIU Z M. Methanol to olefins (MTO): From fundamentals to commercialization[J]. ACS Catal,2015,5(3):1922−1938. doi: 10.1021/acscatal.5b00007
[5]	MARCINIAK A A, ALVES O C, APPEL L G, MOTA J A. Synthesis of dimethyl carbonate from CO₂and methanol over CeO₂: Role of copper as dopant and the use of methyl trichloroacetate as dehydrating agent[J]. J Catal,2019,371(1):88−95.
[6]	YANG Z, FENG J, CHENG H, LIU Y X, JIANG J C. Directional depolymerization of lignin into high added-value chemical with synergistic effect of binary solvents[J]. Bioresour Technol,2021,321(12):124−440.
[7]	LI S, PENG D, YU J. Morphologically controllable Li plating with stable electrochemistry realized in a newly developed DOL-DMM electrolyte system on Au-modified Cu current collector[J]. Ionics,2020,26(8):3979−3988. doi: 10.1007/s11581-020-03527-3
[8]	BADMAEV S D, SMORYGINA A S, PAUKSHTIS E A, BELYAEV V D, SOBYANIN V A, PARMON V N. Gas-phase carbonylation of dimethoxymethane to methyl methoxyacetate on solid acids: The effect of acidity on the catalytic activity[J]. Kinet Catal,2018,59(1):99−103. doi: 10.1134/S0023158418010020
[9]	CHONG J M, SHEN L X. Preparation of chloromethyl methyl ether revisited[J]. Synth Commun,1998,28(15):2801−2806. doi: 10.1080/00397919808004855
[10]	NOUGUIER R, MIGNON V, GRAS J. Synthesis of methylene acetals in the D-glucose, D-galactose, D-mannose, and D-fructose series by an improved transacetalation reaction from dimethoxymethane[J]. Carbohydr Res,1995,277(2):339−345. doi: 10.1016/0008-6215(95)00218-I
[11]	YANG Z, FENG J, CHENG H, LIU Y X, JIAN J C. Directional depolymerization of lignin into high added-value chemical with synergistic effect of binary solvents[J]. Bioresour Technol,2021,321(1):124440.
[12]	WANG J, LIU J, SONG H, CHEN J. Heteropolyacids as efficient catalysts for the synthesis of precursors to ethylene glycol by the liquid-phase carbonylation of dimethoxymethane[J]. Chem Lett,2015,44(6):806−808. doi: 10.1246/cl.150131
[13]	LI M, LONG Y, DENG Z, ZHANG H, YANG X G, WANG G Y. Ruthenium trichloride as a new catalyst for selective production of dimethoxymethane from liquid methanol with molecular oxygen as sole oxidant[J]. Catal Commun,2015,68(4):46−48.
[14]	LIU H C, IGLESIA E. Selective one-step synthesis of dimethoxymethane via methanol or dimethyl ether oxidation on H_3+nV_nMo_12−nPO₄₀ keggin structures[J]. J Phys Chem B,2003,107(39):10840−10847. doi: 10.1021/jp0301554
[15]	FU Y, SHEN J. Selective oxidation of methanol to dimethoxymethane under mild conditions over V₂O₅/TiO₂ with enhanced surface acidity[J]. Chem Commun,2007,21(21):2172−2174.
[16]	TAO M, WANG H, BIN L, ZHAO J X, CAI Q H. Highly selective oxidation of methanol to dimethoxymethane over $ {\rm{SO}}_4^{2 - } $-V₂O₅-ZrO₂[J]. New J Chem,2017,41(16):8370−8376. doi: 10.1039/C7NJ01295K
[17]	CHEN S, MA X. The role of oxygen species in the selective oxidation of methanol to dimethoxymethane over VO_x/TS-1 catalyst[J]. J Ind Eng Chem,2017,45(9):296−300.
[18]	AI M. The production of methyl formate by the vapor-phase oxidation of methanol[J]. J Catal,1982,21(77):279−288.
[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]	ZHANG Z Z, ZHANG Q D, JIA L, WANG W F, SHAO P T, WANG P, HE X, 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,2016,15(6):6109−6117.
[21]	杨奇, 高秀娟, 冯茹, 李明杰, 张俊峰, 张清德, 韩怡卓, 谭猗生. 水热合成的MoO₃-SnO₂催化剂催化氧化二甲醚的性能研究[J]. 燃料化学学报,2019,47(8):934−941. doi: 10.3969/j.issn.0253-2409.2019.08.005 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
[22]	陈文龙, 刘海超. 甲醇选择氧化金属氧化物催化剂的结构与其催化性能的关系[J]. 物理化学学报,2012,28(10):2315−2356. doi: 10.3866/PKU.WHXB201209146 CHEN Wen-long, LIU Hai-chao. Relationship between the structures of metal oxide catalysts and their properties in selective oxidation of methanol[J]. Acta Phys-Chim Sin,2012,28(10):2315−2356. doi: 10.3866/PKU.WHXB201209146
[23]	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.
[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.
[25]	杨奇. 钼锡催化剂上二甲醚低温氧化机理研究[D]. 北京: 中国科学院大学, 2019. 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.
[26]	HANG Z Z, ZHANG Q D, JIA L Y, WANG W F, ZHANG T, HAN Y Z, TSUBAKI N, TAN Y S. Effects f tetrahedral molybdenum oxide species and MoO_x domains on the selective oxidation of dimethyl ther under mild conditions[J]. Catal Sci Technol,2016,6(9):2975−2983. doi: 10.1039/C5CY01569C
[27]	YANG J, XIAO X, CHEN P, ZHU K, CHENG K, YE K, WANG G L, CAO D X, YAN J. Creating oxygen-vacancies in MoO_3−x nanobelts toward high volumetric energy-density asymmetric superercapacitors with long lifespan[J]. Nano Energy,2019,58(1):455−465.