二氧化铈促进钴氧化物表面氧化一氧化碳的原位表征研究

doi:10.1016/S1872-2067(19)63282-1

催化学报 ›› 2019, Vol. 40 ›› Issue (5): 656-663.DOI: 10.1016/S1872-2067(19)63282-1

二氧化铈促进钴氧化物表面氧化一氧化碳的原位表征研究

郇伟伟^a,c, 李洁^a,b, 嵇家辉^c, 邢明阳^c

a 浙江农林大学, 浙江省林业与生物质化学利用重点实验室, 浙江临安 311300;
b 浙江省农业生物资源生化制造协同创新中心, 浙江杭州 310023;
c 华东理工大学化学与分子工程学院, 教育部结构可控先进材料重点实验室, 上海 200237

收稿日期:2018-11-11 修回日期:2018-12-20 出版日期:2019-05-18 发布日期:2019-03-30
通讯作者: 邢明阳
基金资助:
国家重点研发计划（2016YFA0204200）；国家自然科学基金（21822603，21577036，21773062）；上海市浦江人才计划（17PJD011）；中央高校基本科研业务费（22A201514021）；浙江省公益技术研究计划/农村农业（LGN18B010001）；浙江省农业生物资源生物化学协同创新中心（2016KF0005）.

In situ studies on ceria promoted cobalt oxide for CO oxidation

Weiwei Huan^a,c, Jie Li^a,b, Jiahui Ji^c, Mingyang Xing^c

a Zhejiang Provincial Key Laboratory of Chemical Utilization of Forestry Biomass, Zhejiang A & F University, Lin'an 311300, Zhejiang, China;
b Zhejiang provincial Collaborative Innovation Center of Agricultural Biological Resources Biochemical Manufacturing, Hangzhou 310023, Zhejiang, China;
c Key Laboratory for Advanced Materials and Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2018-11-11 Revised:2018-12-20 Online:2019-05-18 Published:2019-03-30
Contact: S1872-2067(19)63282-1
Supported by:
This work was supported by the State Key Research Development Program of China (2016YFA0204200), the National Natural Science Foundation of China (21822603, 21577036, 21773062), the Shanghai Pujiang Program (17PJD011), the Zhejiang public welfare technology research plan/rural agriculture (LGN18B010001), the Zhejiang provincial Collaborative Innovation Center of Agricultural Biological Resources Biochemical Manufacturing (NO:2016KF0005),and the scientific research project of Zhejiang provincial education department (Y201839892).

摘要/Abstract

摘要：

CO氧化由其广泛的应用而成为催化领域中研究的重要反应，Co₃O₄催化剂具有价格低廉、催化活性高等优点而引起研究者的关注，其中，催化剂的结构、表面特性及反应机理等是研究的重点.催化剂的原位研究对观察相变过程，理解相应的表面化学反应和反应机理起着重要的作用.本文采用煅烧法制备了CeO₂掺杂的Co₃O₄，并对其催化CO氧化反应性能进行了研究.通过扫描电镜、高分辨率透射电镜、拉曼光谱和X射线光电子能谱对催化剂的微观结构和形态进行了表征.通过原位X射线衍射（原位XRD）和原位漫反射红外傅立叶变换光谱（原位DRIFTS）表征了CeO₂掺杂Co₃O₄对CO氧化的效果.原位XRD测试是在氢气气氛中进行，借以评估催化剂的氧化还原特性.结果表明，由于CeO₂的补氧能力，CeO₂掺杂可以提高Co²⁺的还原能力，并促进了Co³⁺-Co²⁺-Co³⁺循环.采用原位DRIFTS对CeO₂改性的Co₃O₄表面吸附的碳酸盐物种进行了探究.结果表明，吸附碳酸盐物种的CeO₂掺杂Co₃O₄催化剂的红外峰与纯Co₃O₄相比有所不同.CeO₂掺杂的Co₃O₄上吸附的碳酸盐物种较为活泼，其与催化剂表面的结合作用力比较弱，不会覆盖催化剂表面的活性位点，能有效抑制催化剂的失活.本文揭示了CeO₂掺杂Co₃O₄促进CO氧化的机理，为设计高效氧化CO的催化剂提供了理论支持.
原位XRD的结果表明，由于CeO₂的补氧能力，引入CeO₂可以显著提高Co²⁺的稳定性.换句话说，它可以通过降低Co²⁺的氧化能力来提高Co²⁺的还原能力，有利于促进Co³⁺-Co²⁺-Co³⁺循环的稳定性，从而使Co²⁺更容易转化为Co³⁺.原位DRIFTS表明，在某种程度上，吸附在CeO₂-Co₃O₄表面的碳酸盐物种呈游离态，与催化剂表面的结合作用力较弱.这种类型的碳酸盐更活泼，而且不会像那些强作用在催化剂表面的碳酸盐物种那样使表面钝化.CeO₂-Co₃O₄与Co₃O₄的表面吸附的碳酸盐物种的差异是由于引入的CeO₂对氧化钴表面进行修饰改性的结果.在高温和N₂气氛下进行预处理后，CeO₂表面变得光洁且形成了一些氧空位，其特殊的储氧能力通过弱吸附氧使其表面更加活泼.这些结果证实，经过CeO₂的修饰后，氧化钴表面更加活泼，且更适合CO氧化反应的发生.

关键词: 氧化铈-氧化钴, 一氧化碳氧化, 原位X射线衍射, 原位漫反射红外傅里叶变换光谱学, 碳酸盐物种

Abstract:

In situ studies of catalysts play valuable roles in observing phase transformation, understanding the corresponding surface chemistry and the mechanism of the reaction. In this paper, ceria promoted cobalt oxide was prepared by the calcination method and investigated for the CO oxidation. The microstructure and morphology of CeO₂-Co₃O₄ were investigated by the Scanning Electron Microscope, High-resolution transmission electron microscopy, Raman and X-ray photoelectron spectroscopy characterization. The effect of CeO₂ doping on Co₃O₄ for CO oxidation was characterized by in situ X-ray Diffraction (in situ XRD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). In situ XRD was carried out under H₂ atmosphere to evaluate the redox property of catalysts. The results indicated that the ceria doping can enhance the reducibility of Co²⁺ and promote the Co³⁺-Co²⁺-Co³⁺ cycle, owing to the oxygen replenish property of CeO₂. Furthermore, adsorbed carbonate species on the surface of CeO₂-Co₃O₄ were investigated by in situ-DRIFTS experiment. It was turned out that carbonate species on ceria promoted cobalt oxide catalysts showed different IR peaks compared with pure cobalt oxide. The carbonate species on ceria promoted catalyst are more active, and similar to free state carbonate species with weak bonding to catalyst surface, which can effectively inhibit catalyst inactivation. This study revealed the mechanism of ceria promoting CO oxidation over cobalt oxide, which will provide theoretical support for the design of efficient CO oxidation catalysts.

Key words: CeO₂-Co₃O₄ CO oxidation, In situ X-ray diffraction, In situ diffuse reflectance infrared, Fourier transform spectroscopy, Carbonate species

郇伟伟, 李洁, 嵇家辉, 邢明阳. 二氧化铈促进钴氧化物表面氧化一氧化碳的原位表征研究[J]. 催化学报, 2019, 40(5): 656-663.

Weiwei Huan, Jie Li, Jiahui Ji, Mingyang Xing. In situ studies on ceria promoted cobalt oxide for CO oxidation[J]. Chinese Journal of Catalysis, 2019, 40(5): 656-663.

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二氧化铈促进钴氧化物表面氧化一氧化碳的原位表征研究

In situ studies on ceria promoted cobalt oxide for CO oxidation

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