Effect of molybdenum valence in low Mo/Sn ratio catalysts for the oxidation of methanol to dimethoxymethane

Q3 Energy 燃料化学学报 Pub Date : 2024-01-01 DOI:10.1016/S1872-5813(23)60370-6

Jia WANG , Xiujuan GAO , Faen SONG , Junfeng ZHANG , Xiaoxing WANG , Tao ZHANG , Yisheng TAN , Yizhuo HAN , Qingde ZHANG

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Abstract

A series of Mo/Sn (1:20, molar ratio) catalysts were prepared by two-step hydrothermal synthesis method, and the effect of calcination temperature of tin precursors on the reaction performance of methanol oxidation to dimethoxymethane (DMM) was investigated. The crystal structure, surface properties, redox property and valence change of molybdenum species of the catalyst were characterized by XRD, Raman, FT-IR, XPS, NH₃-TPD and H₂-TPR. The results showed that Mo1Sn20-600°CSn catalyst exhibited better performance than other catalysts, achieving DMM selectivity of 90% with methanol conversion of 30% at 140 °C. From the characterization results, the surface properties of the tin precursors affected the structure of catalyst, the degree of molybdenum oxide dispersion and valence of molybdenum species, and further influenced the performance of the catalysts. The high temperature calcination of tin precursors is more favorable for the generation of Mo⁶⁺ in the Mo1Sn20 catalyst.

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甲醇氧化成二甲氧甲烷的低钼/锑比催化剂中钼价的影响

采用两步水热合成法制备了一系列钼/锡（摩尔比为 1:20）催化剂，并研究了锡前驱体的煅烧温度对甲醇氧化制二甲氧甲烷（DMM）反应性能的影响。通过 XRD、拉曼、傅立叶变换红外光谱、XPS、NH3-TPD 和 H2-TPR 对催化剂的晶体结构、表面性质、氧化还原性质和钼物种的价态变化进行了表征。结果表明，与其他催化剂相比，Mo1Sn20-600°CSn 催化剂表现出更好的性能，在 140 °C 条件下，DMM 选择性达到 90%，甲醇转化率达到 30%。从表征结果来看，锡前驱体的表面性质影响了催化剂的结构、氧化钼的分散程度和钼元素的价态，并进一步影响了催化剂的性能。锡前驱体的高温煅烧更有利于 Mo1Sn20 催化剂中 Mo6+ 的生成。

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.