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

作　　者：Baoling Tian Shujuan Li Shulai Lei Liangxu Lin Wenyue Guo Hao Ren 

机构地区：[1]College of Chemistry and Pharmaceutical Sciences,Qingdao Agricultural University,Qingdao 266109,China [2]Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices,Hubei University of Arts and Science,Xiangyang 441053,China [3]ARC Centre of Excellence for Electromaterials Science,Intelligent Polymer Research Institute,Australia Institute for Innovative Materials(AIIM),Innovation Campus,University of Wollongong,Wollongong 2519,Australia [4]School of Materials Science and Engineering,China University of Petroleum(East China),Qingdao 266580,China

出　　处：《Chinese Chemical Letters》2021年第8期2469-2473,共5页中国化学快报（英文版）

基　　金：financial support from the National Natural Science Foundation of China (NSFC,No.21773309);Highlevel Science Foundation of Qingdao Agricultural University (No.663/1114351);the Fundamental Research Funds for the Central Universities (No.19CX05001A);Hubei University of Arts and Science (No.2020kypytd002);Xiangyang Science and Technology Research and Development (No.2020YL09)。

摘　　要：CO_(2) capture is considered as one of the most ideal strategies for solving the environmental issues and against global warming.Recently,experimental evidence has suggested that aluminum double bond(dialumene) species can capture CO_(2) and further convert it into value-added products.However,the catalytic application of these species is still in its infancy.Both the dynamics mechanism of CO_(2) fixation and the detailed structures of catalytic intermediates are not well understood.In this work,we investigate the structure dependent resonance Raman(RR) signals for different reaction intermediates.Ab-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 process.The unique Raman vibronic feature s contain rich structural information with high temporal resolution,enabling to monitor the transient catalytic intermediates under reaction conditions.Our work shows that RR can be used to monitor intermediates during the dialumene based CO_(2) capture reaction.The 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 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]