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Structural insights of catalytic intermediates in dialumene based CO_(2) capture: Evidences from theoretical resonance Raman spectra

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Chinese Chemical Letters 2021年第8期32卷 2469-2473页

作者： Baoling Tian Shujuan Li Shulai Lei Liangxu Lin Wenyue Guo Hao Ren College of Chemistry and Pharmaceutical Sciences Qingdao Agricultural UniversityQingdao 266109China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and ScienceXiangyang 441053China ARC Centre of Excellence for Electromaterials Science Intelligent Polymer Research InstituteAustralia Institute for Innovative Materials(AIIM)Innovation CampusUniversity of WollongongWollongong 2519Australia School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580China

CO_(2) capture is considered as one of the most ideal strategies for solving the environmental issues and against global ***,experimental evidence has suggested that aluminum double bond(dialumene) species can capture CO_(2) and further convert it into value-added ***,the catalytic application of these species is still in its *** the dynamics mechanism of CO_(2) fixation and the detailed structures of catalytic intermediates are not well *** this work,we investigate the structure dependent resonance Raman(RR) signals for different reaction ***-initio simulations of spontaneous resonance Raman(spRR) and time-domain stimulated resonance Raman(stRR) give spectral signatures correlated to the existence of different intermediates during the CO_(2)-dialumene binding *** unique Raman vibronic feature s contain rich structural information with high temporal resolution,enabling to monitor the transient catalytic intermediates under reaction *** work shows that RR can be used to monitor intermediates during the dialumene based CO_(2) capture *** spectral features not only provide insight into the structural information of intermediate species,but also allow a deeper understanding of the dynamical details of this kind of catalytic process.

关键词： Resonance Raman Ab initio Catalytic intermediate dialumene CO_(2)capture Ultrafast spectroscopy

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