首页|Facet and dual vacancy engineering-boosting BiOBr for enhanced CO2 and epoxide cycloaddition reaction under mild and cocatalyst-free conditions:Double substrate active sites and activated surface bromine ions synergy
Facet and dual vacancy engineering-boosting BiOBr for enhanced CO2 and epoxide cycloaddition reaction under mild and cocatalyst-free conditions:Double substrate active sites and activated surface bromine ions synergy
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Among the many strategies for CO2 resource utilization,the synthetic technology of cyclic carbonates with 100％atom economy through CO2and epoxide is one of the most industrially viable routes,but its efficiency has been severely hampered by the lack of highly active catalytic sites.Moreover,due to the intrinsic thermodynamic stability and kinetic inertia of CO2 and the higher energy barrier of the ring-opening reaction of epoxides,the heterogeneous catalytic conversion of CO2 highly depends on harsh operating conditions,high temperatures and pressures,and the incorporation of cocatalysts.The devel-opment of efficient heterogeneous catalysts for CO2 conversion under cocatalyst-free and mild conditions has always been a challenge.Herein,we have proposed a synergetic strategy of facet and vacancy engi-neering for the construction of highly efficient heterogeneous catalyst BiO1-xBr1-y-(010)for CO2 cycload-dition,where introducing the OVs-BrVs pairs into typical(010)facets BiOBr with simultaneous surface Lewis acid sites Bi3+and nucleophilic sites Br-.By combining theoretical calculations and a series of systematic experiments,such as CO2 temperature-programmed desorption,electron paramagnetic res-onance and fluorescence probe analysis experiments,the introduced OVs-BrVs pair can not only form Bi3+-Bi(3-x)+dual active sites on the surface,which activate PO and CO2 respectively to reduce the energy barrier of CO2 insertion,but also activate Br-near BrVs to enhance their nucleophilic attacking ability and reduce the energy barrier of epoxides ring-opening.As a result,the BiOi-xBr1-y-(010)with abundant surface OVs-BrVs pairs showed a high cyclic carbonates conversion of 99％with 100％selectivity un-der cocatalyst-free and mild conditions,far surpassing most heterogeneous catalytic systems.This work provides a completely new strategy to construct high-performance heterogeneous CO2 cycloaddition cata-lysts through a simple facet and vacancy engineering strategy to overcome the harsh operating conditions limitation and the use of cocatalysts.
CO2 cycloaddition reactionVacancy engineeringFacet engineeringHeterogeneous catalysis
Li Xia、Huanping Chen、Wenzhen Wang、Xingang Jia、Dake Zhang、Li Wang、Panfeng Wu、Leilei Li、Jian Huang
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Shaanxi Engineering Research Center of Green Low-carbon Energy Materials and Processes,College of Chemistry and Chemical Engineering,Xi'an Shiyou University,Xi'an 710065,China
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