催化作用
材料科学
纳米颗粒
炔丙基
三嗪
化学工程
银纳米粒子
卟啉
纳米技术
炔烃
金属有机骨架
有机化学
高分子化学
化学
吸附
工程类
作者
Yiying Yang,Yingyin Li,Zixuan Zhang,Kechi Chen,Rongchang Luo
标识
DOI:10.1021/acsami.3c10521
摘要
The preparation of catalytic hybrid materials by introducing highly dispersed metallic nanoparticles into porous organic polymers (POPs) may be an ideal and promising strategy for integrated CO2 capture and conversion. In terms of the carboxylative cyclization of propargyl alcohols with CO2, the anchoring of silver nanoparticles (AgNPs) on functional POPs to fabricate efficient heterogeneous catalysts is considered to be quite intriguing but remains challenging. In the contribution, well-dispersed AgNPs were successfully anchored onto the porphyrinic triazine-based frameworks by a simple “liquid impregnation and in situ reduction” strategy. The presence of N-rich dual active sites, porphyrin and triazine, which acted as the electron donor and acceptor, respectively, offered a huge opportunity for the nucleation and growth of metal nanoparticles. Significantly, the as-prepared catalyst Ag/TPP-CTF shows excellent catalytic activity (up to 99%) toward the carboxylative cyclization of propargyl alcohols with CO2 at room temperature, achieving record-breaking activities (TOF up to 615 h–1 at 1 bar and 3077 h–1 at 10 bar). Moreover, the catalyst can be easily recovered and reused at least 10 times with retention of high catalytic activity. The possible mechanism involves small-sized AgNP-mediated alkyne activation, which may promote highly efficient and green conversion of CO2. This work paves the way for immobilizing metal nanoparticles onto functional POPs by surface structure changes for enhanced CO2 catalysis.
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