Citation: GAO Xiu-juan, WANG Wen-feng, GU Ying-ying, ZHANG Zhen-zhou, ZHANG Qing-de, HAN Yi-zhuo, TAN Yi-sheng. Performance of SO₄^2-/AC catalysts prepared with different precursors in the synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation[J]. Journal of Fuel Chemistry and Technology, ;2017, 45(9): 1114-1121. shu

Performance of SO₄^2-/AC catalysts prepared with different precursors in the synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation

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

Corresponding author: ZHANG Qing-de, qdzhang@sxicc.ac.cn
Received Date: 11 April 2017
Revised Date: 26 June 2017

Fund Project: the National Natural Science Foundation of China 20903114This work was financially supported by the National Natural Science Foundation of China (21373253, 20903114) and Youth Innovation Promotion Association CAS (2014155)the National Natural Science Foundation of China 21373253Youth Innovation Promotion Association 2014155

Figures(5)

A series of SO₄^2-/AC bifunctional catalysts, in which SO₄^2- and AC acted as the acid sites and redox sites, respectively, are prepared by impregnation with H₂SO₄ and (NH₄)₂SO₄ as precursors and active carbon as support; their catalytic performance in the direct oxidation of dimethyl ether (DME) to polyoxymethylene dimethyl ethers (DMM_x) was investigated. The results show that the catalytic performance of SO₄^2-/AC catalysts is significantly related to the precursor used. Over the 40%H₂SO₄/AC catalyst, the selectivity to DMM_1-2 reaches 59.7%, with a DME conversion of 8.4%; in addition, there is no CO_x observed in the products. However, a large amount of CO_x by-product is formed over the 40%(NH₄)₂SO₄/AC catalyst; meanwhile, the selectivity to DMM is only 2.7% and no DMM₂ is formed. The XRD, N₂ sorption, NH₃-TPD and O₂-TPD-MS characterization results illustrate that the suitable amount of weak acid sites and redox sites of the H₂SO₄/AC catalyst is beneficial to the formation of long chain DMM_x from DME oxidation. The modification of AC with SO₄^2- promotes the activation of O₂ over the surface of AC support, whereas the introduction of H₂SO₄ improves the weak acid sites of the catalyst. On the contrary, the number of medium-strong acid sites of the catalyst is increased by modifying AC with (NH₄)₂SO₄.
- dimethyl ether,
- polyoxymethylene dimethyl ethers,
- direct oxidation,
- precursor,
- SO₄^2-/AC
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沈阳化工大学材料科学与工程学院沈阳 110142

Performance of SO42-/AC catalysts prepared with different precursors in the synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation

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通讯作者: 陈斌, bchen63@163.com

Performance of SO₄^2-/AC catalysts prepared with different precursors in the synthesis of polyoxymethylene dimethyl ethers from dimethyl ether direct oxidation