4.7 Article

From the outside to the inside: Elucidation of the mechanism of pseudomorphic transformation of SBA-15 into MCM-41 by following its time-resolved conversion

期刊

出版社

ELSEVIER
DOI: 10.1016/j.micromeso.2021.111442

关键词

Bimodal mesoporous silica; Pseudomorphic transformation; Mechanism; Complex pore structure; Cavitation

向作者/读者索取更多资源

Pseudomorphic transformation of silica materials is a versatile approach for the fabrication of porous phases, which allows independent control of particle morphology and pore structure. The mechanism and models for the transformation process are still controversial, with pure homogeneous distribution and core-shell models being extreme poles in the debate. Time-resolved conversion of parent silica materials provides insights into the detailed mechanism of pseudomorphic transformation.
Pseudomorphic transformation of silica materials is a versatile approach for the fabrication of porous phases in which the particle morphology and pore structure can be controlled independently from each other. It has been applied already for a wide variety of different parent silica materials, however, there is still a controversy about the details of the mechanism, about the manner of how the transformation proceeds through the body of the particles. The pure homogeneous distribution model on the one hand, and the core-shell model, on the other hand, are the so-to-speak extreme poles in this controversy, not excluding that a mixed-mode model can be valid for a particular parent silica phase. Herein, the detailed mechanism for the pseudomorphic transformation of ordered mesoporous SBA-15 into MCM-41 is elucidated by following the time-resolved conversion of the parent silica material. Upon pseudomorphic transformation, the characteristic morphology of the parent SBA-15 par-ticles remains unchanged, whereas the original pore structure undergoes a successive restructuring in the presence of hexadecyl-trimethylammonium ions as a structure-directing agent. The inflow of the alkaline transformation solution within the pore system of SBA-15 initiates undirected dissolution and re-condensation processes of the pristine pore walls, resulting in an undulation, a slight shrinkage and a partial obstruction of the original mesopores. Simultaneously small domains of MCM-41 with various spatial orientations are formed on the external particle surface, restricting the access to the undulated mesopores within the particle core. The resulting core-shell structure of the partially transformed materials provides interesting gas physisorption hys-teresis phenomena, caused by a cavitation mechanism during the evaporation of adsorbate from partially blocked SBA-15 pores. PXRD reflections that can be assigned to the characteristically large pore spacing of SBA-15 were found within patterns even for materials with a supposedly complete conversion. The occurrence of these reflections can be attributed to inaccessible pore domains of SBA-15. With proceeding transformation, a reduction of the amount of inaccessible SBA-15 pores was observed, finally leading to a material with typical MCM-41 characteristics but with a slightly less pore ordering due to the abrasively conditions during the long hydrothermal treatment.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据