Due to the high local concentration of substrates in confined space, porous solid Bronsted acids have been extensively explored for efficient acid-catalyzed reaction. However, the porous structures with strong Bronste...Due to the high local concentration of substrates in confined space, porous solid Bronsted acids have been extensively explored for efficient acid-catalyzed reaction. However, the porous structures with strong Bronsted acids lack long-term stability due to chemical hydrolysis. Moreover, the products inhibition effect in confined rigid cavities severely obstructs subsequent catalysis. Here, tubular Bronsted acid catalyst with unique recognition of protons was presented by self-assembly of p H-responsive aromatic amphiphiles. The responsive assembly could mechanically transfer hydrogen ions from low-concentration acidic solution into tubular defined pores, thereby producing effective catalytic activity for Mannich reactions in mildly acidic solution. Notably, the tubular catalyst unfolded into flat sheets upon addition of triethylamine for efficient release of products, which could be recovered by subsequent acidification and the catalytic activity still remained. Therefore, the porous Bronsted acid with reversible assembly provides a new strategy for mass synthesis through increasing conversion times.展开更多
基金supported by the Natural Science Foundation of China (No. 21871299)Guangdong Natural Science Funds for Distinguished Young Scholar (No. 2019B151502051)+4 种基金the Fundamental Research Funds for the Central Universities (No.19lgzd21)Guangdong Basic and Applied Basic Research Foundation (No. 2022A1515110991)China Postdocroral Science Foundation (No. 2021M701569)the Open Project of State Key Laboratory of Supramolecular Structure and Materials (Jilin University)the Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University)
文摘Due to the high local concentration of substrates in confined space, porous solid Bronsted acids have been extensively explored for efficient acid-catalyzed reaction. However, the porous structures with strong Bronsted acids lack long-term stability due to chemical hydrolysis. Moreover, the products inhibition effect in confined rigid cavities severely obstructs subsequent catalysis. Here, tubular Bronsted acid catalyst with unique recognition of protons was presented by self-assembly of p H-responsive aromatic amphiphiles. The responsive assembly could mechanically transfer hydrogen ions from low-concentration acidic solution into tubular defined pores, thereby producing effective catalytic activity for Mannich reactions in mildly acidic solution. Notably, the tubular catalyst unfolded into flat sheets upon addition of triethylamine for efficient release of products, which could be recovered by subsequent acidification and the catalytic activity still remained. Therefore, the porous Bronsted acid with reversible assembly provides a new strategy for mass synthesis through increasing conversion times.
