Catalytic oxidation of lignin model non-phenolic monomer Veratryl alcohol over iron containing mesoporous SBA-1

IF 2.5 4区 材料科学 Q2 CHEMISTRY, APPLIED
Nirupama Parida, Paresh Kumar Mohanty, Sharada Shrinivas Pati, Sushanta K. Badamali
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Abstract

Mesoporous solids possessing open framework, tunable pores, high surface area, and considerable thermal stability provide an ideal environment to be employed as solid catalysts, host material, adsorbent, etc. Herein, we report the study about the insertion of iron into the mesoporous silicate framework of SBA-1 and utilize the material as a potential heterogeneous catalyst for the selective oxidation of lignin model non-phenolic monomer, i.e. veratryl alcohol under mild reaction conditions. Veratraldehyde and veratric acid were obtained as the oxidation products. FeSBA-1 in combination with hydrogen peroxide was selective towards veratraldehyde, on the other hand, veratric acid was selectively obtained when tert-butyl hydroperoxide was used as the oxidant under identical reaction conditions. X-ray diffraction pattern of FeSBA-1 revealed the formation of a cubic, three-dimensional SBA-1 structure. HRTEM shows uniform and ordered pore structure having dimensions of ∽ 2.3 ̶ 3.4 nm and wall thickness of ∽ 3.5 nm. FESEM showed regular-shaped FeSBA-1 with spherical morphology having a dimension of ∽ 1.6 μm. BET surface area of 1337 m2 g−1 and pore diameter of ∽ 19 Å was determined by N2 adsorption-desorption measurements. The mesoporous nature of FeSBA-1 was further supported by TGA studies. EPR studies indicated the presence of Fe(III) both in tetrahedral and octahedral coordination within the framework of FeSBA-1. DRUV-VIS studies revealed the presence of Fe(III) in both framework and extra-framework locations of the SBA-1 silicate network. IR studies supported the linkage of Fe–O–Si within FeSBA-1. The absence of the Fe2O3 phase was evidenced by Raman studies.

Abstract Image

Abstract Image

含铁介孔 SBA-1 催化氧化木质素模型非酚类单体 Veratryl 醇
介孔固体具有开放的框架、可调的孔隙、高比表面积和相当高的热稳定性,为用作固体催化剂、宿主材料、吸附剂等提供了理想的环境。在此,我们报告了在 SBA-1 的介孔硅酸盐框架中加入铁的研究,并利用该材料作为一种潜在的异相催化剂,在温和的反应条件下选择性氧化木质素模型非酚类单体(即藜芦醇)。氧化产物为藜芦醛和藜芦酸。在相同的反应条件下,FeSBA-1 与过氧化氢结合对藜芦醛具有选择性,而使用过氧化叔丁酯作为氧化剂时,则可选择性地获得藜芦酸。FeSBA-1 的 X 射线衍射图显示形成了立方三维 SBA-1 结构。HRTEM 显示出均匀有序的孔隙结构,其尺寸为 ∽ 2.3 ̶ 3.4 nm,壁厚为 ∽ 3.5 nm。FESEM 显示,FeSBA-1 形状规则,呈球形,尺寸为 ∽ 1.6 μm。通过对 N2 的吸附-解吸测量,确定其 BET 表面积为 1337 m2 g-1,孔径为 ∽ 19 Å。TGA 研究进一步证实了 FeSBA-1 的介孔性质。EPR 研究表明,FeSBA-1 的框架中存在四面体和八面体配位的 Fe(III)。DRUV-VIS 研究表明,Fe(III) 存在于 SBA-1 硅酸盐网络的框架和框架外位置。红外研究证实了 FeSBA-1 中 Fe-O-Si 的连接。拉曼研究证明不存在 Fe2O3 相。
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来源期刊
Journal of Porous Materials
Journal of Porous Materials 工程技术-材料科学:综合
CiteScore
4.80
自引率
7.70%
发文量
203
审稿时长
2.6 months
期刊介绍: The Journal of Porous Materials is an interdisciplinary and international periodical devoted to all types of porous materials. Its aim is the rapid publication of high quality, peer-reviewed papers focused on the synthesis, processing, characterization and property evaluation of all porous materials. The objective is to establish a unique journal that will serve as a principal means of communication for the growing interdisciplinary field of porous materials. Porous materials include microporous materials with 50 nm pores. Examples of microporous materials are natural and synthetic molecular sieves, cationic and anionic clays, pillared clays, tobermorites, pillared Zr and Ti phosphates, spherosilicates, carbons, porous polymers, xerogels, etc. Mesoporous materials include synthetic molecular sieves, xerogels, aerogels, glasses, glass ceramics, porous polymers, etc.; while macroporous materials include ceramics, glass ceramics, porous polymers, aerogels, cement, etc. The porous materials can be crystalline, semicrystalline or noncrystalline, or combinations thereof. They can also be either organic, inorganic, or their composites. The overall objective of the journal is the establishment of one main forum covering the basic and applied aspects of all porous materials.
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