再分配(选举)
分子筛
路易斯酸
机制(生物学)
化学
化学工程
纳米技术
催化作用
材料科学
计算化学
化学物理
有机化学
物理
工程类
政治学
政治
量子力学
法学
作者
Miao Yu,Sai Geng,Qingle Zhao,Yuhao Nie,Pengpeng Wen,Mingming Han,Anyang Shi,Jingyi Lao,Jialuo Yin,Yue Liu,Huihui Wang,Shiwei Liu
标识
DOI:10.1021/acssuschemeng.5c01903
摘要
The precise regulation of multistep reaction paths in the synthesis of 2-ethylanthraquinone, with lower yields due to contradictions in the stability of intermediates and compatibility of active sites, poses a great challenge to industrial production. In this study, an electron redistribution strategy is proposed: By anchoring the active metal gallium to the Hβ molecular sieve framework, a Lewis and Brønsted acid pair that can dynamically adapt the reaction path is constructed. Based on the Friedel–Crafts acylation reaction, it was revealed that the Ga 3+ center undergoes a valence transition during the catalytic process, which synergizes with the Brønsted acidic site (Si–OH-Al) to regulate the adsorption configuration of the intermediates, and improves the catalytic efficiency of the modified Hβ molecular sieves. Compared to the conventional sulfuric acid method ( E = 5.2), a yield of 89.3% was achieved with an E coefficient of 0.8, a reduction of 85%. By optimizing the reaction temperature to 250 °C (300 °C for the acid-catalyzed method), energy consumption was reduced by 37%, while sulfonation waste was reduced by 1.6 tons per ton of product. The hierarchical pore structure of Ga–Hβ enhanced molecular diffusion efficiency, reducing activation energy by 35% (40.07 kJ·mol –1 for Ga–Hβ vs 62.11 kJ·mol –1 for H 2 SO 4 ) and enabling four stable regeneration cycles with 80% activity retention. It provides a universal theoretical framework for space-time regulation of multistep catalytic networks in complex organic synthesis and provides a new direction for industrial catalytic synthesis of 2-ethylanthraquinones.
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