Hydroxyl and amino dual-functionalized core-shell molecular sieves featuring hydrogen bond donor groups for efficient CO2 cycloaddition.

[Display omitted] • Core-shell catalysts (mSiO 2 @MCM-NH 2 -OH) prove the confirmed to have –OH, –NH 2 /Br-. • Double HBD groups and Lewis base synergize to promote CO 2 cycloaddition reaction. • After 10 cycles of mSiO 2 @MCM-NH 2 -OH, the yield remained at 93%. • A synergistic catalysis mechanism was confirmed by theoretical calculations. In CO 2 cycloaddition reactions, hydrogen bond donor (HBD) groups are considered environmentally friendly substitutes for metals to promote epoxide ring-opening through interactions with nucleophilic anions. A core-shell structured ILs-based catalyst (mSiO 2 @MCM-NH 2 -OH) with dual hydrogen bond donors (–OH and –NH 2) was synthesized by copolymerization strategy. Through in-depth characterization, it has been demonstrated that the catalyst (mSiO 2 @MCM-NH 2 -OH) possesses multiple catalytic active sites including –OH, –NH 2 , Br- groups, and the synergistic effect of double HBD groups (–OH and –NH 2) and Lewis base (Br-) significantly improved the catalytic activity. Meanwhile, the core-shell structure of the catalyst effectively prevents the loss of active components, which makes the yield remain at about 94 % after 10 cycles. Based on Density Functional Theory (DFT) calculations, a synergistic catalytic mechanism, which involves dual hydrogen-bond donors (–OH and –NH 2) and Lewis bases (Br-) was proposed. The cooperative interaction between –OH/–NH 2 and Br- reduced the ring-opening barrier of epoxide from 58.6 to 32.0 kcal mol−1 significantly, and thereby facilitated the CO 2 cycloaddition reaction. [ABSTRACT FROM AUTHOR]