α-和γ-环糊精改性法制备的Ni/SBA-15催化剂的物化性质及其在甲烷二氧化碳重整中的催化性能

引用本文: 刘会敏, 李宇明, 吴昊, 刘佳雄, 贺德华. α-和γ-环糊精改性法制备的Ni/SBA-15催化剂的物化性质及其在甲烷二氧化碳重整中的催化性能[J]. 催化学报, 2015, 36(3): 283-289. doi: 10.1016/S1872-2067(14)60242-4 shu

Citation: Huimin Liu, Yuming Li, Hao Wu, Jiaxiong Liu, Dehua He. Effects of α- and γ-cyclodextrin-modified impregnation method on physicochemical properties of Ni/SBA-15 and its catalytic performance in CO₂ reforming of methane[J]. Chinese Journal of Catalysis, 2015, 36(3): 283-289. doi: 10.1016/S1872-2067(14)60242-4 shu

α-和γ-环糊精改性法制备的Ni/SBA-15催化剂的物化性质及其在甲烷二氧化碳重整中的催化性能

通讯作者: 贺德华

摘要: 以多羟基有机物α-或γ-环糊精为分散促进剂制备了Ni/SBA-15催化剂, 通过N₂吸附-脱附、X射线衍射、透射电镜、程序升温还原和热重等手段对该催化剂的物理化学性质进行了表征, 并将其应用于甲烷二氧化碳重整(CRM)制合成气反应. 结果显示, 与采用传统浸渍法制备的Ni/SBA-15催化剂相比, 采用α-或γ-环糊精改性法制备的催化剂具有更小的NiO颗粒, 并在CRM中显示出更高的催化活性及更强的抗积碳性能. 机理研究表明, 采用传统浸渍法制备Ni/SBA-15催化剂时, 浸渍液中的Ni²⁺主要在浓度梯度的作用下逐渐进入到SBA-15孔道内部, Ni²⁺水合物容易团聚, 分散程度较低; 而采用α-或γ-环糊精改性方法制备催化剂时, 在水溶液中Ni²⁺与环糊精形成包覆物, 环糊精携带Ni²⁺进入SBA-15孔道内, 并且环糊精的存在使得Ni²⁺之间相互隔离, 以高度分散形态存在于SBA-15孔道表面, 有利于后续热处理中NiO在载体上较好地分散.

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English

Effects of α- and γ-cyclodextrin-modified impregnation method on physicochemical properties of Ni/SBA-15 and its catalytic performance in CO₂ reforming of methane

1.
Innovative Catalysis Program, Key Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, China

Corresponding author: 贺德华

Received Date: 14 September 2014
Available Online: 20 March 2015

Abstract: Organic compounds containing multiple hydroxyl groups, namely α-cyclodextrin and γ-cyclodextrin, were used as additives for promoting Ni dispersion on supported Ni/SBA-15 catalysts. Catalysts prepared using modified and unmodified impregnation methods were characterized using N₂ adsorption-desorption isotherms, X-ray diffraction, transmission electron microscopy, temperature-programmed reduction, and thermogravimetric analysis, and their catalytic performance in the CO₂ reforming of methane (CRM) to syngas was evaluated. The results show that compared with Ni/SBA-15 prepared using a conventional impregnation method, the cyclodextrin-modified catalysts had smaller NiO particles. They also exhibited higher catalytic activity and had stronger ability to resist carbon deposition in the CRM. Mechanistic studies showed that for the unmodified catalysts, Ni²⁺ could migrate into the channels of SBA-15 as a result of concentration differences, and the Ni species were sintered during the following thermal treatment processes, and could not be well dispersed. In contrast, various types of complex were formed between Ni(NO₃)₂ and the cyclodextrins, and this would be favorable for Ni²⁺ being taken into the channels of the SBA-15. The presence of cyclodextrins was beneficial to the mutual isolation of Ni species, and finally resulted in better dispersion of Ni species.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

α-和γ-环糊精改性法制备的Ni/SBA-15催化剂的物化性质及其在甲烷二氧化碳重整中的催化性能

通讯作者: 贺德华

English

Effects of α- and γ-cyclodextrin-modified impregnation method on physicochemical properties of Ni/SBA-15 and its catalytic performance in CO₂ reforming of methane

Corresponding author: 贺德华

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

α-和γ-环糊精改性法制备的Ni/SBA-15催化剂的物化性质及其在甲烷二氧化碳重整中的催化性能

通讯作者: 贺德华

English

Effects of α- and γ-cyclodextrin-modified impregnation method on physicochemical properties of Ni/SBA-15 and its catalytic performance in CO2 reforming of methane

Corresponding author: 贺德华

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

Effects of α- and γ-cyclodextrin-modified impregnation method on physicochemical properties of Ni/SBA-15 and its catalytic performance in CO₂ reforming of methane

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs