Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM
Abstract In bimetallic heterostructured nanoparticles (NPs), the synergistic effect between their different metallic components leads to higher catalytic activity compared to the activity of the individual components. However, how the dynamic changes through which these NPs adopt catalytically activ...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2022-06-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202105599 |
| _version_ | 1811248006437011456 |
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| author | Tanmay Ghosh Xiangwen Liu Wenming Sun Meiqi Chen Yuxi Liu Yadong Li Utkur Mirsaidov |
| author_facet | Tanmay Ghosh Xiangwen Liu Wenming Sun Meiqi Chen Yuxi Liu Yadong Li Utkur Mirsaidov |
| author_sort | Tanmay Ghosh |
| collection | DOAJ |
| description | Abstract In bimetallic heterostructured nanoparticles (NPs), the synergistic effect between their different metallic components leads to higher catalytic activity compared to the activity of the individual components. However, how the dynamic changes through which these NPs adopt catalytically active structures during a reaction and how the restructuring affects their activity are largely unknown. Here, using operando transmission electron microscopy, structural changes are studied in bimetallic Ni–Rh NPs, comprising of a Ni core whose surface is decorated with smaller Rh NPs, during a CO oxidation reaction. The direct atomic‐scale imaging reveals that, under O2‐rich conditions, Ni core partially transforms into NiO, forming a (Ni+NiO)–Rh hollow nanocatalyst with high catalytic activity. Under O2‐poor conditions, Rh NPs alloy with the surface of the core to form a NiRh‐alloy surface, and the NPs display significantly lower activity. The theoretical calculations indicate that NiO component that forms only under O2‐rich conditions enhances the activity by preventing the CO poisoning of the nanocatalysts. The results demonstrate that visualizing the structural changes during reactions is indispensable in identifying the origin of catalytic activity. These insights into the dynamic restructuring of NP catalysts under a reactive environment are critical for the rational design of high‐performance nanocatalysts. |
| first_indexed | 2024-04-12T15:19:31Z |
| format | Article |
| id | doaj.art-6854b0ff9b8a46328aff88d299aec9ae |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-04-12T15:19:31Z |
| publishDate | 2022-06-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-6854b0ff9b8a46328aff88d299aec9ae2022-12-22T03:27:30ZengWileyAdvanced Science2198-38442022-06-01917n/an/a10.1002/advs.202105599Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEMTanmay Ghosh0Xiangwen Liu1Wenming Sun2Meiqi Chen3Yuxi Liu4Yadong Li5Utkur Mirsaidov6Department of Physics National University of Singapore Singapore 117551 SingaporeDepartment of Physics National University of Singapore Singapore 117551 SingaporeCollege of Science China Agricultural University Beijing 100193 P. R. ChinaCollege of Environmental and Energy Engineering Beijing University of Technology Beijing 100124 P. R. ChinaCollege of Environmental and Energy Engineering Beijing University of Technology Beijing 100124 P. R. ChinaDepartment of Chemistry Tsinghua University Beijing 100084 P. R. ChinaDepartment of Physics National University of Singapore Singapore 117551 SingaporeAbstract In bimetallic heterostructured nanoparticles (NPs), the synergistic effect between their different metallic components leads to higher catalytic activity compared to the activity of the individual components. However, how the dynamic changes through which these NPs adopt catalytically active structures during a reaction and how the restructuring affects their activity are largely unknown. Here, using operando transmission electron microscopy, structural changes are studied in bimetallic Ni–Rh NPs, comprising of a Ni core whose surface is decorated with smaller Rh NPs, during a CO oxidation reaction. The direct atomic‐scale imaging reveals that, under O2‐rich conditions, Ni core partially transforms into NiO, forming a (Ni+NiO)–Rh hollow nanocatalyst with high catalytic activity. Under O2‐poor conditions, Rh NPs alloy with the surface of the core to form a NiRh‐alloy surface, and the NPs display significantly lower activity. The theoretical calculations indicate that NiO component that forms only under O2‐rich conditions enhances the activity by preventing the CO poisoning of the nanocatalysts. The results demonstrate that visualizing the structural changes during reactions is indispensable in identifying the origin of catalytic activity. These insights into the dynamic restructuring of NP catalysts under a reactive environment are critical for the rational design of high‐performance nanocatalysts.https://doi.org/10.1002/advs.202105599CO oxidationheterogeneous catalysisnanoparticlesoperando TEM |
| spellingShingle | Tanmay Ghosh Xiangwen Liu Wenming Sun Meiqi Chen Yuxi Liu Yadong Li Utkur Mirsaidov Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM Advanced Science CO oxidation heterogeneous catalysis nanoparticles operando TEM |
| title | Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM |
| title_full | Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM |
| title_fullStr | Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM |
| title_full_unstemmed | Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM |
| title_short | Revealing the Origin of Low‐Temperature Activity of Ni–Rh Nanostructures during CO Oxidation Reaction with Operando TEM |
| title_sort | revealing the origin of low temperature activity of ni rh nanostructures during co oxidation reaction with operando tem |
| topic | CO oxidation heterogeneous catalysis nanoparticles operando TEM |
| url | https://doi.org/10.1002/advs.202105599 |
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