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Operando study of palladium nanoparticles inside UiO-67 MOF for catalytic hydrogenation of hydrocarbons
Faraday Discussions ( IF 3.3 ) Pub Date : 2018-01-22 , DOI: 10.1039/c7fd00224f A. L. Bugaev 1, 2, 3, 4, 5 , Alexander A. Guda 1, 2, 3, 4 , Kirill A. Lomachenko 6, 7, 8 , Elizaveta G. Kamyshova 1, 2, 3, 4 , Mikhail A. Soldatov 1, 2, 3, 4 , Gurpreet Kaur 5, 9, 10, 11, 12 , Sigurd Øien-Ødegaard 5, 9, 10, 11, 12 , Luca Braglia 1, 2, 3, 4, 5 , Andrea Lazzarini 5, 9, 10, 11, 12 , Maela Manzoli 13, 14, 15, 16 , Silvia Bordiga 5, 14, 15, 16, 17 , Unni Olsbye 5, 9, 10, 11, 12 , Karl P. Lillerud 5, 9, 10, 11, 12 , Alexander V. Soldatov 1, 2, 3, 4 , Carlo Lamberti 1, 2, 3, 4, 18
Faraday Discussions ( IF 3.3 ) Pub Date : 2018-01-22 , DOI: 10.1039/c7fd00224f A. L. Bugaev 1, 2, 3, 4, 5 , Alexander A. Guda 1, 2, 3, 4 , Kirill A. Lomachenko 6, 7, 8 , Elizaveta G. Kamyshova 1, 2, 3, 4 , Mikhail A. Soldatov 1, 2, 3, 4 , Gurpreet Kaur 5, 9, 10, 11, 12 , Sigurd Øien-Ødegaard 5, 9, 10, 11, 12 , Luca Braglia 1, 2, 3, 4, 5 , Andrea Lazzarini 5, 9, 10, 11, 12 , Maela Manzoli 13, 14, 15, 16 , Silvia Bordiga 5, 14, 15, 16, 17 , Unni Olsbye 5, 9, 10, 11, 12 , Karl P. Lillerud 5, 9, 10, 11, 12 , Alexander V. Soldatov 1, 2, 3, 4 , Carlo Lamberti 1, 2, 3, 4, 18
Affiliation
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Functionalization of metal–organic frameworks with metal nanoparticles (NPs) is a promising way for producing advanced materials for catalytic applications. We present the synthesis and in situ characterization of palladium NPs encapsulated inside a functionalized UiO-67 metal–organic framework. The initial structure was synthesized with 10% of PdCl2bpydc moieties with grafted Pd ions replacing standard 4,4′-biphenyldicarboxylate linkers. This material exhibits the same high crystallinity and thermal stability of standard UiO-67. Formation of palladium NPs was initiated by sample activation in hydrogen and monitored by in situ X-ray powder diffraction and X-ray absorption spectroscopy (XAS). The reduction of PdII ions to Pd0 occurs above 200 °C in 6% H2/He flow. The formed palladium NPs have an average size of 2.1 nm as limited by the cavities of UiO-67 structure. The resulting material showed high activity towards ethylene hydrogenation. Under reaction conditions, palladium was found to form a carbide structure indicated by operando XAS, while formation of ethane was monitored by mass spectroscopy and infra-red spectroscopy.
中文翻译：
Operando钯纳米颗粒的UIO-67 MOF内的碳氢化合物的催化加氢研究
用金属纳米颗粒（NPs）对金属有机框架进行功能化是生产用于催化应用的先进材料的一种有前途的方法。我们介绍了封装在功能化的UiO-67金属有机框架内的钯NP的合成和原位表征。初始结构由10％的PdCl 2 bpydc部分合成，其中接枝的Pd离子取代了标准的4,4'-联苯二羧酸酯连接基。这种材料具有与标准UiO-67相同的高结晶度和热稳定性。钯NP的形成是通过氢气中的样品活化引发的，并通过原位X射线粉末衍射和X射线吸收光谱法（XAS）进行监控。将Pd II离子还原为Pd在6％H 2 / He流中，高于200°C发生0。所形成的钯NP的平均尺寸为2.1 nm，受UiO-67结构腔的限制。所得材料显示出对乙烯氢化的高活性。在反应条件下，发现钯形成了由操作XAS指示的碳化物结构，同时通过质谱和红外光谱监测了乙烷的形成。
更新日期：2018-09-03
中文翻译：
Operando钯纳米颗粒的UIO-67 MOF内的碳氢化合物的催化加氢研究
用金属纳米颗粒（NPs）对金属有机框架进行功能化是生产用于催化应用的先进材料的一种有前途的方法。我们介绍了封装在功能化的UiO-67金属有机框架内的钯NP的合成和原位表征。初始结构由10％的PdCl 2 bpydc部分合成，其中接枝的Pd离子取代了标准的4,4'-联苯二羧酸酯连接基。这种材料具有与标准UiO-67相同的高结晶度和热稳定性。钯NP的形成是通过氢气中的样品活化引发的，并通过原位X射线粉末衍射和X射线吸收光谱法（XAS）进行监控。将Pd II离子还原为Pd在6％H 2 / He流中，高于200°C发生0。所形成的钯NP的平均尺寸为2.1 nm，受UiO-67结构腔的限制。所得材料显示出对乙烯氢化的高活性。在反应条件下，发现钯形成了由操作XAS指示的碳化物结构，同时通过质谱和红外光谱监测了乙烷的形成。
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