Composition dependent selectivity of bimetallic Au-Pd NPs immobilised on titanate nanotubes in catalytic oxidation of glucose

Motaz Khawaji; Yiming Zhang; Melody Loh; Inês Graça; Ecaterina Ware; David Chadwick

doi:10.1016/j.apcatb.2019.117799

Composition dependent selectivity of bimetallic Au-Pd NPs immobilised on titanate nanotubes in catalytic oxidation of glucose

Motaz Khawaji, Yiming Zhang, Melody Loh, Inês Graça, Ecaterina Ware, David Chadwick^*

^*Corresponding author for this work

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

19 Citations (Scopus)

Abstract

The catalytic performance of Au-Pd nanoparticles (NP) prepared by colloidal synthesis and immobilised on titanate nanotubes (Ti-NT) in the selective oxidation of glucose to gluconic and glucaric acids has been studied under initially basic and relatively mild conditions. Catalysts with varying compositions displayed quite different product selectivity especially in relation to deeper oxidation. The yield of glucaric acid was found to be proportional to the atomic content of Au in the Au-Pd NPs: Au/Ti-NT exhibited the highest selectivity to glucaric acid, while Au₁₅Pd₈₅/Ti-NT displayed the highest selectivity to gluconic acid, S_GLO > 98%. Catalyst recycling revealed deactivation, which appears to be due to a combination of metal leaching, particle size changes and product adsorption, and is associated with the gradual fall in pH of the reaction mixture. Results suggest that the leached Au species play a significant role in the oxidation of gluconic to glucaric acid.

Original language	English
Article number	117799
Journal	Applied Catalysis B: Environmental
Volume	256
Early online date	31 May 2019
DOIs	https://doi.org/10.1016/j.apcatb.2019.117799
Publication status	Published - 5 Nov 2019

Keywords

Au-Pd
Glucose
Selective oxidation
Sol-Immobilisation
Titanate nanotubes

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title = "Composition dependent selectivity of bimetallic Au-Pd NPs immobilised on titanate nanotubes in catalytic oxidation of glucose",

abstract = "The catalytic performance of Au-Pd nanoparticles (NP) prepared by colloidal synthesis and immobilised on titanate nanotubes (Ti-NT) in the selective oxidation of glucose to gluconic and glucaric acids has been studied under initially basic and relatively mild conditions. Catalysts with varying compositions displayed quite different product selectivity especially in relation to deeper oxidation. The yield of glucaric acid was found to be proportional to the atomic content of Au in the Au-Pd NPs: Au/Ti-NT exhibited the highest selectivity to glucaric acid, while Au15Pd85/Ti-NT displayed the highest selectivity to gluconic acid, SGLO > 98%. Catalyst recycling revealed deactivation, which appears to be due to a combination of metal leaching, particle size changes and product adsorption, and is associated with the gradual fall in pH of the reaction mixture. Results suggest that the leached Au species play a significant role in the oxidation of gluconic to glucaric acid.",

keywords = "Au-Pd, Glucose, Selective oxidation, Sol-Immobilisation, Titanate nanotubes",

author = "Motaz Khawaji and Yiming Zhang and Melody Loh and In{\^e}s Gra{\c c}a and Ecaterina Ware and David Chadwick",

note = "Motaz Khawaji gratefully acknowledges the financial support of Saudi Aramco. This work was funded by EPSRC EP/K014749/1. We thank Katty Elizabeth Cabezas Ter{\'a}n for assistance with preliminary measurements on glucose oxidation, and Babajide Aina and Li Lyu for help in carrying out some of the catalytic activity measurements on salicyl alcohol. We are grateful to Professor Graham Hutchings and Dr. Robert Armstrong from Cardiff Catalysis Institute for providing us with a sample of glucaric acid. ",

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T1 - Composition dependent selectivity of bimetallic Au-Pd NPs immobilised on titanate nanotubes in catalytic oxidation of glucose

AU - Khawaji, Motaz

AU - Zhang, Yiming

AU - Loh, Melody

AU - Graça, Inês

AU - Ware, Ecaterina

AU - Chadwick, David

N1 - Motaz Khawaji gratefully acknowledges the financial support of Saudi Aramco. This work was funded by EPSRC EP/K014749/1. We thank Katty Elizabeth Cabezas Terán for assistance with preliminary measurements on glucose oxidation, and Babajide Aina and Li Lyu for help in carrying out some of the catalytic activity measurements on salicyl alcohol. We are grateful to Professor Graham Hutchings and Dr. Robert Armstrong from Cardiff Catalysis Institute for providing us with a sample of glucaric acid.

PY - 2019/11/5

Y1 - 2019/11/5

N2 - The catalytic performance of Au-Pd nanoparticles (NP) prepared by colloidal synthesis and immobilised on titanate nanotubes (Ti-NT) in the selective oxidation of glucose to gluconic and glucaric acids has been studied under initially basic and relatively mild conditions. Catalysts with varying compositions displayed quite different product selectivity especially in relation to deeper oxidation. The yield of glucaric acid was found to be proportional to the atomic content of Au in the Au-Pd NPs: Au/Ti-NT exhibited the highest selectivity to glucaric acid, while Au15Pd85/Ti-NT displayed the highest selectivity to gluconic acid, SGLO > 98%. Catalyst recycling revealed deactivation, which appears to be due to a combination of metal leaching, particle size changes and product adsorption, and is associated with the gradual fall in pH of the reaction mixture. Results suggest that the leached Au species play a significant role in the oxidation of gluconic to glucaric acid.

AB - The catalytic performance of Au-Pd nanoparticles (NP) prepared by colloidal synthesis and immobilised on titanate nanotubes (Ti-NT) in the selective oxidation of glucose to gluconic and glucaric acids has been studied under initially basic and relatively mild conditions. Catalysts with varying compositions displayed quite different product selectivity especially in relation to deeper oxidation. The yield of glucaric acid was found to be proportional to the atomic content of Au in the Au-Pd NPs: Au/Ti-NT exhibited the highest selectivity to glucaric acid, while Au15Pd85/Ti-NT displayed the highest selectivity to gluconic acid, SGLO > 98%. Catalyst recycling revealed deactivation, which appears to be due to a combination of metal leaching, particle size changes and product adsorption, and is associated with the gradual fall in pH of the reaction mixture. Results suggest that the leached Au species play a significant role in the oxidation of gluconic to glucaric acid.

KW - Au-Pd

KW - Glucose

KW - Selective oxidation

KW - Sol-Immobilisation

KW - Titanate nanotubes

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Composition dependent selectivity of bimetallic Au-Pd NPs immobilised on titanate nanotubes in catalytic oxidation of glucose

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