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(Reference retrieved automatically from Web of Science through information on FAPESP grant and its corresponding number as mentioned in the publication by the authors.)

Exploring the multifunctionality and accessibility of vanadosilicates to produce acrylic acid in one-pot glycerol oxydehydration

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Author(s):
Vieira, Luiz H. [1, 2] ; Lopez-Castillo, Alejandro [3] ; Jones, Christopher W. [1] ; Martins, Leandro [2]
Total Authors: 4
Affiliation:
[1] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 - USA
[2] Sao Paulo State Univ UNESP, Inst Chem, R Prof Francisco Degni 55, BR-14800900 Araraquara, SP - Brazil
[3] Univ Fed Sao Carlos, Dept Chem, Rod Washington Luis, Km 235, BR-13565905 Sao Carlos, SP - Brazil
Total Affiliations: 3
Document type: Journal article
Source: APPLIED CATALYSIS A-GENERAL; v. 602, JUL 25 2020.
Web of Science Citations: 0
Abstract

Acrylic acid is one of the most attractive products directly produced from glycerol, and many efforts are still made to thoroughly understand the role of different catalytic sites in the reaction. In this work, we prepared Al-free vanadosilicates presenting structures analog to ferrierite and ITQ-6 zeolites (2D and 3D structures). The materials were efficient in catalyzing the one-pot conversion of glycerol to acrylic acid. The different vanadium species in the catalysts had specific roles in each step of the reaction. By exposing samples to humid conditions, dissociative adsorption of water produced hydroxylated sites (O3V-OH-Si) that acted as extrinsic Bronsted acid sites. The deprotonation energy of these sites was estimated by DFT calculations and found to be close to deprotonation energy of intrinsic Bronsted acidity of aluminosilicates with the same zeolitic structure, indicating the ability of the active site to dehydrate glycerol to acrolein. The formation of these sites seems to effectively block potential Lewis acidity of the vanadosilicates since acetol, a dehydration side product, was not formed. Spectroscopic data showed changes in oxidation states of vanadium in these sites after the reaction, presenting V5+ and V4+ states, indicating the activity of these sites on the oxidation step during oxidation of acrolein to acrylic acid. By decreasing vanadium content during synthesis, delamination to ITQ-6 was more effective, increasing accessibility and, consequently, the productivity of sites. (AU)

FAPESP's process: 18/01258-5 - Novel chemical catalytic and photocatalytic processes for the direct conversion of methane and CO2 to products
Grantee:José Maria Correa Bueno
Support Opportunities: Research Projects - Thematic Grants
FAPESP's process: 17/00860-0 - A study on selective oxidation of methanol over lamellar vanadosilicates catalysts
Grantee:Luiz Henrique Vieira
Support Opportunities: Scholarships abroad - Research Internship - Doctorate
FAPESP's process: 19/12501-0 - Theoretical study of bidimensional systems
Grantee:Alejandro López Castillo
Support Opportunities: Regular Research Grants
FAPESP's process: 19/17156-0 - Strategies for improving the activity of catalysts based on vanadium oxides prepared by various methods for application in oxidation reactions
Grantee:Leandro Pierroni Martins
Support Opportunities: Regular Research Grants
FAPESP's process: 14/20116-6 - Development and application of lamellar vanadosilicates as catalysts in the glycerol oxidative dehydration
Grantee:Luiz Henrique Vieira
Support Opportunities: Scholarships in Brazil - Doctorate