钾调变Mo/SBA-15催化剂用于乙烷选择氧化制乙醛

引用本文: 李建梅, 刘坚, 任立伟, 刘清龙, 赵震, 韦岳长, 段爱军, 姜桂元. 钾调变Mo/SBA-15催化剂用于乙烷选择氧化制乙醛[J]. 物理化学学报, 2014, 30(9): 1736-1744. doi: 10.3866/PKU.WHXB201407091 shu

Citation: LI Jian-Mei, LIU Jian, REN Li-Wei, LIU Qing-Long, ZHAO Zhen, WEI Yue-Chang, DUAN Ai-Jun, JIANG Gui-Yuan. Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts[J]. Acta Physico-Chimica Sinica, 2014, 30(9): 1736-1744. doi: 10.3866/PKU.WHXB201407091 shu

钾调变Mo/SBA-15催化剂用于乙烷选择氧化制乙醛

基金项目:
国家自然科学基金（21376261，21173270，21177160)

北京市自然科学基金（2142027)

国家高技术研究发展计划项目（863）（2013AA065302)

高等学校博士学科点专项科研基金项目（20130007110007）资助

摘要:

采用两步浸渍法制备钾改性的Mo/SBA-15 催化剂. 采用N₂吸附，X射线衍射（XRD），透射电镜（TEM），紫外-可见（UV-Vis）吸收光谱，拉曼（Raman）光谱，NH₃程序升温脱附（NH₃-TPD），CO₂程序升温脱附（CO₂-TPD），H₂程序升温还原（H₂-TPR）等手段表征催化剂的物理化学性质. 研究结果表明，在Mo_0.75/SBA-15 中添加K之后，有新物种钾钼酸盐生成，并且当K/Mo的摩尔比不同时，钼物种的存在状态也不同. 添加钾之后，催化剂的活性和总醛（甲醛、乙醛、丙烯醛）的选择性均有所提高，并且受钾的添加量影响. 在575 ℃时，在K_0.25-Mo_0.75/SBA-15催化剂上醛的收率可高达8.5%（摩尔分数）.

关键词:

English

Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts

1.
State Key Laboratory of Heavy Oil, College of Science, China University of Petroleum, Beijing 102249, P. R. China
Received Date: 16 April 2014
Available Online: 29 August 2014
Fund Project:
国家自然科学基金（21376261，21173270，21177160)

北京市自然科学基金（2142027)

国家高技术研究发展计划项目（863）（2013AA065302)

高等学校博士学科点专项科研基金项目（20130007110007）资助

Abstract:

Potassium-modified SBA-15-supported molybdenum oxide catalysts were prepared using a twostep impregnation method. The physical and chemical properties of the catalysts were characterized using N2- adsorption-desorption, X-ray diffraction (XRD), transmission electron microscope (TEM), UV-visible (UV-Vis) spectroscopy, Raman spectroscopy, NH₃ temperature-programmed desorption (NH₃-TPD), CO₂ temperatureprogrammed desorption (CO₂-TPD), and H₂ temperature-programmed reduction (H₂-TPR). The results showed that potassium addition resulted in the formation of new potassium molybdates, and the states of molybdenum species varied with changes in the K/Mo molar ratio. The addition of potassium to Mo_0.75/SBA-15 effectively improved the activity of catalysts and the selectivity to the total aldehydes (formaldehyde, acetaldehyde, and acrolein), especially for acetaldehyde in the selective oxidation of ethane. The turn-over frequency (TOF) and product selectivity depended strongly on the potassium content. The maximum selectivity and yield of aldehydes were obtained by varying the K/Mo molar ratio. At 575 ℃, the maximum yield of aldehydes reached 8.5%(molar fraction) over K_0.25-Mo_0.75/SBA-15 catalyst. The formation of new potassium-molybdates promoted the activities and selectivities of the catalysts.

Key words:

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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

钾调变Mo/SBA-15催化剂用于乙烷选择氧化制乙醛

English

Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

钾调变Mo/SBA-15催化剂用于乙烷选择氧化制乙醛

English

Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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