文献类型：期刊文献

英文题名：Engineering synergistic Br?nsted–Lewis sites in MFI zeolite via atomic niobium dispersion for selective alkylation to durene

作者：Shi, Jialun[1]; Liu, Yuncai[1]; Pu, Xin[1]; Han, Xin[1]; Ye, Lei[1]; Qin, Xinglong[3]; Zhang, Hongbin[4]; Liu, Jichang[1,2]

机构：[1] State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003, China; [3] State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao, 266580, China; [4] Key Laboratory of Silicate Cultural Heritage Conservation [Ministry of Education], Institute for the Conservation of Cultural Heritage, School of Cultural Heritage and Information Management, Shanghai University, Shanghai, 200444, China

年份：2026

卷号：541

外文期刊名：Chemical Engineering Journal

收录：EI(收录号：20260159150)

语种：英文

外文关键词：Acidity - Atoms - Bromine compounds - Catalyst activity - Catalyst selectivity - Dispersions - Niobium - Niobium compounds

摘要：The selective alkylation of 1,2,4-trimethylbenzene (pseudocumene) to durene represents a pivotal route for C9 aromatic valorization, yet it is constrained by an inherent activity-selectivity-stability trade-off in conventional HZSM-5 catalysts. Herein, we break this limitation by engineering synergistic Br?nsted and Lewis acid sites within an MFI zeolite via the atomic dispersion of low-loading niobium (Nb). A one-step hydrothermal method successfully incorporates Nb into the framework, creating isolated Nb sites with an average coordination number of ～4.8. This unique structure generates medium-strength acidity and a balanced Br?nsted-to-Lewis acid ratio, which are crucial for the selective methylation pathway. The optimized catalyst (Nb/Si ≈ 5.67‰) achieves a remarkable 1,2,4-trimethylbenzene conversion of 39.0% with 58.2% durene selectivity (98.0% among tetramethylbenzenes) and a high space-time yield of 704.7 mg·gcat?1·h?1 under optimal conditions (390 °C, 0.8 MPa). Comprehensive characterization and stability tests confirm the structural integrity and regenerability of the catalyst. This work demonstrates a rational design strategy for zeolite catalysts through precise heteroatom modulation, offering broad implications for aromatic upgrading and related tandem processes. ? 2026 Elsevier B.V.