TY - JOUR
T1 - Pt Nanoparticles on Beta zeolites for Catalytic Toluene Oxidation
T2 - Effect of the Hydroxyl Groups of Beta Zeolite**
AU - Zou, Run
AU - Chansai, Sarayute
AU - Xu, Shaojun
AU - An, Bing
AU - Zainal, Shima
AU - Zhou, Yangtao
AU - Xin, Ruojia
AU - Gao, Pan
AU - Hou, Guangjin
AU - D'Agostino, Carmine
AU - Holmes, Stuart M.
AU - Hardacre, Christopher
AU - Jiao, Yilai
AU - Fan, Xiaolei
N1 - Publisher Copyright:
© 2023 The Authors. ChemCatChem published by Wiley-VCH GmbH.
PY - 2023/11/8
Y1 - 2023/11/8
N2 - Stabilisation of metal species using hydroxyl-rich dealuminated zeolites is a promising method for catalysis. However, insights into the interactions between the hydroxyl groups in zeolite and noble metals and their effects on catalysis are not yet fully understood. Herein, comparative studies were conducted using Pt catalysts supported on hydroxyl-rich dealuminated Beta (deAl-Beta) and the pristine proton-form Beta (H-Beta) for catalytic oxidation of toluene. The findings suggest that during impregnation the Pt precursor (i. e., Pt(NH3)4(NO3)2) interacted with different sites on deAl-Beta and H-Beta, leading to the formation of supported Pt nanoparticles with different physicochemical properties. In detail, for H-Beta, the Pt precursor interacted with Al-OH and isolated external Si-OH sites, yielding Pt NPs with a higher Pt0 proportion of ~71 % compared to ~57 % Pt0 on deAl-Beta. Comparatively, abundant hydroxyl groups on deAl-Beta such as silanol nest and isolated internal Si-OH stabilised highly active Pt-O species. The resulting Pt/deAl-Beta exhibited improved activity and anti-coking ability than Pt/H-Beta in catalytic toluene oxidation. For example, the temperature for 50 % toluene conversion was 193 °C for Pt/deAl-Beta vs. 232 °C for Pt/H-Beta, and the coke deposition was 1.7 % vs. 6.7 % (after the 24-h longevity test), respectively. According to the toluene-temperature programmed desorption (toluene-TPD), 1H nuclear magnetic resonance (1H NMR) relaxation and in situ diffuse reflection Fourier transform spectroscopy (in situ DRIFTS) characterisation, the enhanced performance of Pt/deAl-Beta could be ascribed to (i) the active Pt-O sites stabilised by hydroxyl groups, which interact with toluene easily for conversion, and (ii) the acid-free feature of the deAl-Beta support, which avoids the formation of coke precursors (such as benzoate species) on the catalyst surface. Findings of the work can serve as the design guidelines for making effective supported metal catalysts using zeolitic carriers.
AB - Stabilisation of metal species using hydroxyl-rich dealuminated zeolites is a promising method for catalysis. However, insights into the interactions between the hydroxyl groups in zeolite and noble metals and their effects on catalysis are not yet fully understood. Herein, comparative studies were conducted using Pt catalysts supported on hydroxyl-rich dealuminated Beta (deAl-Beta) and the pristine proton-form Beta (H-Beta) for catalytic oxidation of toluene. The findings suggest that during impregnation the Pt precursor (i. e., Pt(NH3)4(NO3)2) interacted with different sites on deAl-Beta and H-Beta, leading to the formation of supported Pt nanoparticles with different physicochemical properties. In detail, for H-Beta, the Pt precursor interacted with Al-OH and isolated external Si-OH sites, yielding Pt NPs with a higher Pt0 proportion of ~71 % compared to ~57 % Pt0 on deAl-Beta. Comparatively, abundant hydroxyl groups on deAl-Beta such as silanol nest and isolated internal Si-OH stabilised highly active Pt-O species. The resulting Pt/deAl-Beta exhibited improved activity and anti-coking ability than Pt/H-Beta in catalytic toluene oxidation. For example, the temperature for 50 % toluene conversion was 193 °C for Pt/deAl-Beta vs. 232 °C for Pt/H-Beta, and the coke deposition was 1.7 % vs. 6.7 % (after the 24-h longevity test), respectively. According to the toluene-temperature programmed desorption (toluene-TPD), 1H nuclear magnetic resonance (1H NMR) relaxation and in situ diffuse reflection Fourier transform spectroscopy (in situ DRIFTS) characterisation, the enhanced performance of Pt/deAl-Beta could be ascribed to (i) the active Pt-O sites stabilised by hydroxyl groups, which interact with toluene easily for conversion, and (ii) the acid-free feature of the deAl-Beta support, which avoids the formation of coke precursors (such as benzoate species) on the catalyst surface. Findings of the work can serve as the design guidelines for making effective supported metal catalysts using zeolitic carriers.
KW - Beta zeolite
KW - Pt nanoparticles
KW - dealumination
KW - hydroxyl groups
KW - toluene oxidation
UR - http://www.scopus.com/inward/record.url?scp=85174615276&partnerID=8YFLogxK
U2 - 10.1002/cctc.202300811
DO - 10.1002/cctc.202300811
M3 - Article
AN - SCOPUS:85174615276
SN - 1867-3880
VL - 15
JO - ChemCatChem
JF - ChemCatChem
IS - 21
M1 - e202300811
ER -