Catalytic performance of bulk and colloidal Co/Al layered double hydroxide with Au nanoparticles in aerobic olefin oxidation

Sónia R. Leandro; Cristina I. Fernandes; A. S. Viana; A. C. Mourato; Pedro D. Vaz; Carla D. Nunes

doi:10.1016/j.apcata.2019.117155

Catalytic performance of bulk and colloidal Co/Al layered double hydroxide with Au nanoparticles in aerobic olefin oxidation

Sónia R. Leandro, Cristina I. Fernandes, A. S. Viana, A. C. Mourato, Pedro D. Vaz, Carla D. Nunes

Research output: Contribution to journal › Article › peer-review

13 Citations (Scopus)

Abstract

A Co/Al layered double hydroxide material was synthesized in both bulk and exfoliated (colloidal) forms. Anion exchange with methionine allowed immobilization of Au nanoparticles previously prepared by a biomimetic method using an anti-oxidant tea aqueous extract to reduce the Au salt solution. The catalytic performance of bulk and exfoliated clays Au-hybrid materials was assessed in aerobic olefin epoxidation. Both catalysts were very active towards the epoxide products and with very interesting substrate conversion levels after 80 h reaction time. The Au-exfoliated material, where the nanosheets work as large ligands, yielded higher product stereoselectivity in the case of limonene epoxidation. This arises from a confined environment around the Au nanoparticles wrapped by the clay nanosheets modulating access to the catalytic active centres by reagents. Mechanistic assessment was also accomplished for styrene oxidation by DFT methods.

Original language	English
Article number	117155
Journal	Applied Catalysis A: General
Volume	584
DOIs	https://doi.org/10.1016/j.apcata.2019.117155
Publication status	Published - 25 Aug 2019
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2019 Elsevier B.V.

Funding

The authors would like to acknowledge Fundação para a Ciência e a Tecnologia (FCT), Portugal for financial support (project UID/MULTI/00612/2013). CIF (SFRH/BD/81029/2011) and AM (SFRH/BPD/35036/2007) also acknowledge FCT for financial support. G09 calculations were made possible due to the computing resources provided by STFC Scientific Computing Department's SCARF cluster. We also thank the reviewers for raising pertinent questions that contributed largely to improve this manuscript. The authors would like to acknowledge Fundação para a Ciência e a Tecnologia (FCT), Portugal for financial support (project UID/MULTI/00612/2013 ). CIF ( SFRH/BD/81029/2011 ) and AM ( SFRH/BPD/35036/2007 ) also acknowledge FCT for financial support. G09 calculations were made possible due to the computing resources provided by STFC Scientific Computing Department's SCARF cluster. We also thank the reviewers for raising pertinent questions that contributed largely to improve this manuscript.

Funders	Funder number
Science and Technology Facilities Council
Fundação para a Ciência e a Tecnologia	SFRH/BD/81029/2011, UID/MULTI/00612/2013, SFRH/BPD/35036/2007

Keywords

Aerobic oxidation catalysis
Amino acids
Clays
Gold nanoparticles

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10.1016/j.apcata.2019.117155

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title = "Catalytic performance of bulk and colloidal Co/Al layered double hydroxide with Au nanoparticles in aerobic olefin oxidation",

abstract = "A Co/Al layered double hydroxide material was synthesized in both bulk and exfoliated (colloidal) forms. Anion exchange with methionine allowed immobilization of Au nanoparticles previously prepared by a biomimetic method using an anti-oxidant tea aqueous extract to reduce the Au salt solution. The catalytic performance of bulk and exfoliated clays Au-hybrid materials was assessed in aerobic olefin epoxidation. Both catalysts were very active towards the epoxide products and with very interesting substrate conversion levels after 80 h reaction time. The Au-exfoliated material, where the nanosheets work as large ligands, yielded higher product stereoselectivity in the case of limonene epoxidation. This arises from a confined environment around the Au nanoparticles wrapped by the clay nanosheets modulating access to the catalytic active centres by reagents. Mechanistic assessment was also accomplished for styrene oxidation by DFT methods.",

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AU - Leandro, Sónia R.

AU - Fernandes, Cristina I.

AU - Viana, A. S.

AU - Mourato, A. C.

AU - Vaz, Pedro D.

AU - Nunes, Carla D.

PY - 2019/8/25

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N2 - A Co/Al layered double hydroxide material was synthesized in both bulk and exfoliated (colloidal) forms. Anion exchange with methionine allowed immobilization of Au nanoparticles previously prepared by a biomimetic method using an anti-oxidant tea aqueous extract to reduce the Au salt solution. The catalytic performance of bulk and exfoliated clays Au-hybrid materials was assessed in aerobic olefin epoxidation. Both catalysts were very active towards the epoxide products and with very interesting substrate conversion levels after 80 h reaction time. The Au-exfoliated material, where the nanosheets work as large ligands, yielded higher product stereoselectivity in the case of limonene epoxidation. This arises from a confined environment around the Au nanoparticles wrapped by the clay nanosheets modulating access to the catalytic active centres by reagents. Mechanistic assessment was also accomplished for styrene oxidation by DFT methods.

AB - A Co/Al layered double hydroxide material was synthesized in both bulk and exfoliated (colloidal) forms. Anion exchange with methionine allowed immobilization of Au nanoparticles previously prepared by a biomimetic method using an anti-oxidant tea aqueous extract to reduce the Au salt solution. The catalytic performance of bulk and exfoliated clays Au-hybrid materials was assessed in aerobic olefin epoxidation. Both catalysts were very active towards the epoxide products and with very interesting substrate conversion levels after 80 h reaction time. The Au-exfoliated material, where the nanosheets work as large ligands, yielded higher product stereoselectivity in the case of limonene epoxidation. This arises from a confined environment around the Au nanoparticles wrapped by the clay nanosheets modulating access to the catalytic active centres by reagents. Mechanistic assessment was also accomplished for styrene oxidation by DFT methods.

KW - Aerobic oxidation catalysis

KW - Amino acids

KW - Clays

KW - Gold nanoparticles

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Catalytic performance of bulk and colloidal Co/Al layered double hydroxide with Au nanoparticles in aerobic olefin oxidation

Abstract

Bibliographical note

Funding

Keywords

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