首页|Crystal facet-dependent CO2 cycloaddition to epoxides over ZnO catalysts

Crystal facet-dependent CO2 cycloaddition to epoxides over ZnO catalysts

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With regard to green chemistry and sustainable development,the fixation of CO2 into epoxides to form cyclic carbonates is an attractive and promising pathway for CO2 utilization.Metal oxides,renowned as promising eco-friendly catalysts for industrial production,are often undervalued in terms of their impact on the CO2 addition reaction.In this work,we successfully developed ZnO nanoplates with(002)surfaces and ZnO nanorods with(100)surfaces via morphology-oriented regulation to explore the effect of crystal faces on CO2 cycloaddition.The quantitative data obtained from electron paramagnetic resonance spectroscopy indicated that the concentration of oxygen vacancies on the ZnO nanoplate surfaces was more than twice that on the ZnO nanorod surfaces.Density functional theory calculations suggested that the(002)surfaces have lower adsorption energies for CO2 and epichlorohydrin than the(100)surfaces.As a result,the yield of cyclochloropropene carbonate on the ZnO nanoplates(64.7％)was much greater than that on the ZnO nanorods(42.3％).Further evaluation of the reused catalysts revealed that the decrease in the oxygen vacancy concentration was the primary factor contributing to the decrease in catalytic performance.Based on these findings,a possible catalytic mechanism for CO2 cycloaddition with epichlorohydrin was proposed.This work provides a new idea for the controllable preparation of high-performance ZnO catalysts for the synthesis of cyclic carbonates from CO2 and epoxides.

carbon dioxidecycloadditionzinc oxidecrystal faceoxygen vacancy

Yongjian Wei、Ying Li、Yunfei Xu、Yinghui Sun、Tong Xu、Haiou Liang、Jie Bai

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Inner Mongolia Key Laboratory of Industrial Catalysis,Hohhot 010051,China

College of Chemical Engineering,Inner Mongolia University of Technology,Hohhot 010051,China

国家自然科学基金内蒙古自然科学基金内蒙古自然科学基金Foundation of Inner Mongolia Education DepartmentProgram for Young Talents of Science and Technology of Inner Mongolia

220081772023MS020042023MS02011JY20220266NJYT23040

2024

10.1007/s11705-024-2412-6

化学科学与工程前沿
高等教育出版社

化学科学与工程前沿

CSTPCDEI
影响因子：0.172
ISSN：2095-0179
年,卷(期)：2024.18(5)
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