Mahouche-Chergui, Samia, Oun, Abdallah, Haddadou, Imane, Hoyez, Clémentine, Michely, Laurent, Ouellet-Plamondon, Claudiane et Carbonnier, Benjamin.
2021.
« Efficient and recyclable heterogeneous catalyst based on PdNPs stabilized on a green-synthesized graphene-like nanomaterial: Effect of surface functionalization ».
ACS Applied Materials and Interfaces, vol. 13, nº 37.
pp. 44673-44685.
Compte des citations dans Scopus : 3.
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Résumé
A straightforward and efficient approach was reported to surface functionalize graphene-like nanomaterial with abundant carboxylic acid groups for anchoring palladium nanoparticles with a highly increased stability and their use as highly active and stable heterogeneous catalyst for the reduction of both cationic (methylene blue, MB) and anionic (eosin-Y, Eo-Y) toxic organic dyes. The large specific surface area (SBET = 266.94 m2/g) graphene-like nanomaterial (GHN) was prepared through green and cost-effective pyrolysis process from saccharose using layered bentonite clay as a template. To introduce a high density of carboxylic acid functions, GHN nanomaterial was first doubly functionalized by successive grafting of (3- glycidyloxypropyl)trimethoxysilane (GPTMS) and tris(4-hydroxyphenyl)methane triglycidyl ether (TGE) using two different approaches. The GHN nanomaterial functionalized with more epoxide functions was then selected for further functionalization with carboxylic acid functions via a ring-opening reaction through a two-step hydrolysis (H2SO4)/oxidation (KMnO4) approach. The GHN nanomaterial bearing carboxylic acid groups was then treated with sodium hydroxide to produce deprotonated carboxylic acid-rich support. Finally, GHN-COO- binds strongly a high density of Pd2+ ions to form stable complexes which after reduction by NaBH4 leads to highly dispersed, densely anchored and uniformly distributed PdNPs on the surface of the functionalized GHN. The obtained GHN-COO@PdNPs nanohybrid revealed an excellent catalytic activity in the reduction of MB and Eo-Y by an excess of NaBH4 at room temperature with pseudo first-order rate constant (kapp) values of 1.65 x 10-2 and 0.93 x 10-2 s-1, respectively. In addition, the obtained results indicated that the as-synthesized catalyst exhibited excellent recyclability showing more than 94% conversion of MB dye even after eight consecutive runs. The high catalytic performance can be attributed to the high dispersion, stability, and no leaching of the GHN-supported PdNPs, which undoubtedly resulted from the efficiency of the GHN surface functionalization. Moreover, the high reactivity of the epoxy groups grafted onto GHN makes it versatile sustainable platform for the formation and stabilization of metallic nanoparticles of different nature leading to promising heterogeneous nanocatalysts for a broad range of catalytic reactions.
| Type de document: | Article publié dans une revue, révisé par les pairs |
|---|---|
| Professeur: | Professeur Ouellet-Plamondon, Claudiane |
| Affiliation: | Génie de la construction |
| Date de dépôt: | 13 oct. 2021 16:31 |
| Dernière modification: | 22 janv. 2025 18:26 |
| URI: | https://espace2.etsmtl.ca/id/eprint/23283 |
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