@article{Zhang2026, 
author = {Mengting Zhang and Zhihao Chen and Jie Feng and Wenfeng Lang and Yongheng Jia and Peng Yuan and Xiaopeng Min and Yujia Zhang and Jingjing Zhao and Lang Wu and Li Han and Zhikun Peng},
title = {Diethanolamine-assisted construction of a hierarchical zeolite framework for enhanced diffusion and transformation of key intermediates in tandem catalysis},
year = {2026},
journal = {Nano Research},
volume = {19},
number = {8},
pages = {94908673},
keywords = {bifunctional catalysis, hierarchical zeolites, intermediate diffusion, acid site accessibility, metal-acid cooperation.},
url = {https://www.sciopen.com/article/10.26599/NR.2026.94908673},
doi = {10.26599/NR.2026.94908673},
abstract = {Rational design of metal-acid bifunctional catalysts is crucial for steering selectivity in tandem catalysis, yet conventional metal/zeolite systems often suffer from diffusion-imposed limitations that hinder intermediate transport. Herein, we report a diethanolamine-assisted alkaline treatment (DEA-AT) strategy to reconstruct β zeolite into a hierarchical framework featuring radially aligned, exterior-connected mesoporous channels (β-DEA-AT). This architecture markedly improved the accessibility of intermediate cyclohexene to Brønsted acid sites and strengthened metal-acid cooperation in benzene hydroalkylation. As a result, Ru/β-DEA-AT catalysts delivered markedly enhanced performance, achieving a cyclohexylbenzene yield of 35.2%, benzene conversion of 62.1%, and a formation rate of 49.6 mmolCHB·gcat−1·h−1, surpassing both conventionally alkali-treated Ru/β-AT (30.6% conversion, 11.6% CHB yield, 31.0 mmolCHB·gcat−1·h−1) and pristine Ru/β catalysts (33.1% conversion, 21.6% CHB yield, 30.5 mmolCHB·gcat−1·h−1). Systematic investigations revealed that the DEA-induced hierarchical reconstruction facilitated the rapid migration of cyclohexene intermediates within the zeolite framework, as reflected by an increase in the apparent cyclohexene diffusion coefficient from 1.81 × 10−5 cm2·s−1 for Ru/β100 to 6.42 × 10−5 cm2·s−1 for Ru/β100-DEA-AT, where shortened diffusion pathways and enhanced accessibility of Brønsted acid sites promote intermediate transport and transformation. These findings establish pore-environment engineering as a generalizable strategy to regulate intermediate transformations through metal-acid synergy, providing guidance for the design of next-generation multifunctional tandem catalysts.}
}