SBA-15负载高分散纳米NiO的丙烷氧化脱氢制丙烯催化性能

引用本文: 鲁怀乾, 石磊, 何冲, 翁维正, 黄传敬, 万惠霖. SBA-15负载高分散纳米NiO的丙烷氧化脱氢制丙烯催化性能[J]. 物理化学学报, 2012, 28(11): 2697-2704. doi: 10.3866/PKU.WHXB201207091 shu

Citation: LU Huai-Qian, SHI Lei, HE Chong, WENG Wei-Zheng, HUANG Chuan-Jing, WAN Hui-Lin. Highly-Dispersed NiO Nanoparticles on SBA-15 for Oxidative Dehydrogenation of Propane to Propylene[J]. Acta Physico-Chimica Sinica, 2012, 28(11): 2697-2704. doi: 10.3866/PKU.WHXB201207091 shu

SBA-15负载高分散纳米NiO的丙烷氧化脱氢制丙烯催化性能

基金项目:
国家重点基础研究发展计划(973) (2010CB732303) (973) (2010CB732303)

国家自然科学基金(21173173, 21073148, 21033006) (21173173, 21073148, 21033006)

教育部创新团队项目(IRT1036) (IRT1036)

福建省重大科技专项(2009HZ0002-1)资助项目 (2009HZ0002-1)

摘要:

采用浸渍法通过改变焙烧气氛制备了系列NiO/SBA-15 (w_NiO=20%)催化剂, 并考察了催化剂的丙烷氧化脱氢(ODHP)反应性能. 实验结果表明, 与在静止和流动空气中焙烧的催化剂相比, 在1%NO/He (V_NO/V_He=1:99)气氛中焙烧的NiO/SBA-15-NO具有优异的低温丙烷氧化脱氢制丙烯性能, 在350 ℃时, 丙烷的转化率和丙烯收率分别约达29%和13%. 反应温度升至450 ℃时, 丙烯的选择性仍保持在45%左右. X射线粉末衍射(XRD)和透射电镜(TEM)测试结果表明, 1%NO/He气氛可有效抑制焙烧过程中NiO纳米颗粒的团聚, 使NiO物种高分散于SBA-15 的孔道中. H₂-程序升温还原(H₂-TPR)和O₂-程序升温脱附(O₂-TPD)测试结果表明, 随着NiO在SBA-15上分散度的提高, 催化剂的抗还原性增强, ODHP活性氧物种O-的含量增加, 进而使1%NO/He气氛中焙烧的NiO/SBA-15-NO在较宽的温度范围内(350-450 ℃)均具有良好的丙烯选择性, 并显著提高了催化剂的低温活性.

关键词:

NiO/SBA-15
/ 丙烷
/ 氧化脱氢
/ 丙烯
/ 焙烧气氛

English

Highly-Dispersed NiO Nanoparticles on SBA-15 for Oxidative Dehydrogenation of Propane to Propylene

1.
State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Labo-ratory for Green Chemical Productions of Alcohols, Ethers and Esters, Department of Chem-istry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China
Received Date: 25 May 2012
Available Online: 17 October 2012
Fund Project:
国家重点基础研究发展计划(973) (2010CB732303)

国家自然科学基金(21173173, 21073148, 21033006)

教育部创新团队项目(IRT1036)

福建省重大科技专项(2009HZ0002-1)资助项目

Abstract:

A series of NiO/SBA-15 (w_NiO=20%) catalysts were prepared by impregnating SBA-15 with an aqueous solution of nickel nitrate followed by calcining under three different atmospheres. The resulting materials were studied with regard to the oxidative dehydrogenation of propane (ODHP) to propylene. Compared to the catalysts calcined under either static or moving air, the NiO/SBA-15-NO catalyst calcined under flowing 1%NO/He (V_NO/V_He=1:99) atmosphere demonstrated greater activity for this reaction at low temperature. Propylene yield of ~13% with propane conversion of ~29% was obtained at 350 ℃ and the propylene selectivity remained at about 45% even when the reaction temperature was raised to 450 ℃. X-ray diffraction (XRD), transmission electron microscopy (TEM), H₂-temperature program reduction (H₂-TPR), and O₂-temperature program desorption (O₂-TPD) characterizations were used to investigate the intrinsic differences between these NiO/SBA-15 catalysts. It was found that NiO species in the catalyst calcined under 1%NO/He atmosphere were highly dispersed inside the mesopores of SBA-15. With the increasing of NiO dispersion on the support, the quantity of NiO species with a reduction temperature above 450 ℃ increased significantly. In addition, the density of O-species on the catalyst calcined under 1%NO/He was much higher than that in the case of the other two samples. These factors are responsible for the superior performance of the NiO/SBA-15-NO catalyst for the ODHP reaction over the temperature range 350 to 450 ℃.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

SBA-15负载高分散纳米NiO的丙烷氧化脱氢制丙烯催化性能

English

Highly-Dispersed NiO Nanoparticles on SBA-15 for Oxidative Dehydrogenation of Propane to Propylene

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

SBA-15负载高分散纳米NiO的丙烷氧化脱氢制丙烯催化性能

English

Highly-Dispersed NiO Nanoparticles on SBA-15 for Oxidative Dehydrogenation of Propane to Propylene

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

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