Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications
It is well-established that the inclusion of small atomic species such as boron (B) in powder metal catalysts can subtly modify catalytic properties, and the associated changes in the metal lattice imply that the B atoms are located in the interstitial sites. However, there is no compelling evidence...
| Auteurs principaux: | , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Journal article |
| Langue: | English |
| Publié: |
American Chemical Society
2019
|
| _version_ | 1826257171791216640 |
|---|---|
| author | Chen, T Ellis, I Hooper, T Liberti, E Ye, L Lo, B O'Leary, C Sheader, A Martinez, G Jones, L Ho, P Zhao, P Cookson, J Bishop, P Chater, P Hanna, J Nellist, P Tsang, S |
| author_facet | Chen, T Ellis, I Hooper, T Liberti, E Ye, L Lo, B O'Leary, C Sheader, A Martinez, G Jones, L Ho, P Zhao, P Cookson, J Bishop, P Chater, P Hanna, J Nellist, P Tsang, S |
| author_sort | Chen, T |
| collection | OXFORD |
| description | It is well-established that the inclusion of small atomic species such as boron (B) in powder metal catalysts can subtly modify catalytic properties, and the associated changes in the metal lattice imply that the B atoms are located in the interstitial sites. However, there is no compelling evidence for the occurrence of interstitial B atoms, and there is a concomitant lack of detailed structural information describing the nature of this occupancy and its effects on the metal host. In this work, we use an innovative combination of high-resolution 11B magic-angle-spinning (MAS) and 105Pd static solid-state NMR nuclear magnetic resonance (NMR), synchrotron X-ray diffraction (SXRD), in situ X-ray pair distribution function (XPDF), scanning transmission electron microscopy-annular dark field imaging (STEM-ADF), electron ptychography, and electron energy loss spectroscopy (EELS) to investigate the B atom positions, properties, and structural modifications to the palladium lattice of an industrial type interstitial boron doped palladium nanoparticle catalyst system (Pd-intB/C NPs). In this study, we report that upon B incorporation into the Pd lattice, the overall face centered cubic (FCC) lattice is maintained; however, short-range disorder is introduced. The 105Pd static solid-state NMR illustrates how different types (and levels) of structural strain and disorder are introduced in the nanoparticle history. These structural distortions can lead to the appearance of small amounts of local hexagonal close packed (HCP) structured material in localized regions. The short-range lattice tailoring of the Pd framework to accommodate interstitial B dopants in the octahedral sites of the distorted FCC structure can be imaged by electron ptychography. This study describes new toolsets that enable the characterization of industrial metal nanocatalysts across length scales from macro- to microanalysis, which gives important guidance to the structure-activity relationship of the system. |
| first_indexed | 2024-03-06T18:13:54Z |
| format | Journal article |
| id | oxford-uuid:03f1268c-b140-478f-a444-ff18cd6b0b06 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T18:13:54Z |
| publishDate | 2019 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:03f1268c-b140-478f-a444-ff18cd6b0b062022-03-26T08:49:08ZInterstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modificationsJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:03f1268c-b140-478f-a444-ff18cd6b0b06EnglishSymplectic Elements at OxfordAmerican Chemical Society2019Chen, TEllis, IHooper, TLiberti, EYe, LLo, BO'Leary, CSheader, AMartinez, GJones, LHo, PZhao, PCookson, JBishop, PChater, PHanna, JNellist, PTsang, SIt is well-established that the inclusion of small atomic species such as boron (B) in powder metal catalysts can subtly modify catalytic properties, and the associated changes in the metal lattice imply that the B atoms are located in the interstitial sites. However, there is no compelling evidence for the occurrence of interstitial B atoms, and there is a concomitant lack of detailed structural information describing the nature of this occupancy and its effects on the metal host. In this work, we use an innovative combination of high-resolution 11B magic-angle-spinning (MAS) and 105Pd static solid-state NMR nuclear magnetic resonance (NMR), synchrotron X-ray diffraction (SXRD), in situ X-ray pair distribution function (XPDF), scanning transmission electron microscopy-annular dark field imaging (STEM-ADF), electron ptychography, and electron energy loss spectroscopy (EELS) to investigate the B atom positions, properties, and structural modifications to the palladium lattice of an industrial type interstitial boron doped palladium nanoparticle catalyst system (Pd-intB/C NPs). In this study, we report that upon B incorporation into the Pd lattice, the overall face centered cubic (FCC) lattice is maintained; however, short-range disorder is introduced. The 105Pd static solid-state NMR illustrates how different types (and levels) of structural strain and disorder are introduced in the nanoparticle history. These structural distortions can lead to the appearance of small amounts of local hexagonal close packed (HCP) structured material in localized regions. The short-range lattice tailoring of the Pd framework to accommodate interstitial B dopants in the octahedral sites of the distorted FCC structure can be imaged by electron ptychography. This study describes new toolsets that enable the characterization of industrial metal nanocatalysts across length scales from macro- to microanalysis, which gives important guidance to the structure-activity relationship of the system. |
| spellingShingle | Chen, T Ellis, I Hooper, T Liberti, E Ye, L Lo, B O'Leary, C Sheader, A Martinez, G Jones, L Ho, P Zhao, P Cookson, J Bishop, P Chater, P Hanna, J Nellist, P Tsang, S Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title | Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title_full | Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title_fullStr | Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title_full_unstemmed | Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title_short | Interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst: properties and structural modifications |
| title_sort | interstitial boron atoms in the palladium lattice of an industrial type of nanocatalyst properties and structural modifications |
| work_keys_str_mv | AT chent interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT ellisi interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT hoopert interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT libertie interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT yel interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT lob interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT olearyc interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT sheadera interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT martinezg interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT jonesl interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT hop interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT zhaop interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT cooksonj interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT bishopp interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT chaterp interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT hannaj interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT nellistp interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications AT tsangs interstitialboronatomsinthepalladiumlatticeofanindustrialtypeofnanocatalystpropertiesandstructuralmodifications |