文献类型：期刊文献

英文题名：Al-Modified Dendritic Fibrous Nanosilica Catalyst: Accurately Regulated Acidity for Tunable Product Distribution in 1-Decene Oligomerization

作者：Zhou, Yousheng[1];Liu, Chuanlei[1];Li, Peicheng[1];Wang, Yifan[1];Zhao, Qiyue[1];Jiang, Hao[1];Wu, Qiumin[1];Shen, Benxian[1];Sun, Hui[1,2];Han, Xuejiao[3]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Xinjiang Univ, Sch Chem Engn & Technol, Minist Key Lab Oil & Gas Fine Chem, Urumqi 830046, Peoples R China;[3]SHCCIG Yulin Chem Co Ltd, Xian 719302, Peoples R China

年份：2025

卷号：15

期号：12

起止页码：10286

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20252418578671);WOS:【SCI-EXPANDED(收录号:WOS:001500770600001)】；

基金：This work is financially supported by Key R&D Project in the Xinjiang Uygur Autonomous Region (2024B01018) and the National Natural Science Foundation of China (Grants 21878097 and 22178109).

语种：英文

外文关键词：1-decene; oligomerization; heterogeneous catalysis; dendritic fibrous nanosilica; acid strength

摘要：Olefin oligomerization plays a pivotal role in producing value-added chemicals and functional materials, driving the development of the chemical industry. Acid catalysts are widely utilized in olefin oligomerization, yet precisely controlling acidity remains a significant challenge due to the considerable difficulties in regulating the complex coordination of the active components with the supports. In this study, a series of Al-modified dendritic fibrous nanosilica catalysts (Al-DFNS) were synthesized and applied in the oligomerization of 1-decene to polyalphaolefins (PAOs). Multiple characterizations elucidate that the hydrogen-replaced Al-DFNS (H-Al-DFNS) featured a unique three-dimensional center-radial channel with hierarchical pores, while pulsed-field gradient nuclear magnetic resonance (PFG-NMR) further indicates that the high density of accessible acidic sites and diffusion-limited pore properties lead to much higher catalytic efficiency than diverse siliceous catalysts. Acid distribution measurement and product analysis together reveal that H-Al-DFNS has a well-balanced ratio of Br & oslash;nsted acid sites (BAS) to Lewis acid sites (LAS). Specifically, high acid strength enhances hydrogen transfer and contributes to high selectivity of trimer and reduced dimer production. Density functional theory (DFT) calculation highlights the crucial role of the stability of carbocation intermediates on acid sites in the oligomerization reaction. The present work provides a reliable strategy for accurately regulated acidity for tunable oligomerization product distribution and initiates the applications of a kind of promising catalytic material in olefin oligomerization.