Deciphering the Role of Vinylene Carbonate in Shaping CO2 Cluster Growth and Stability via Wavelet-Enhanced Microwave Spectroscopy

IF 15.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-02-03 DOI:10.1021/jacs.4c14584

Chenxu Wang, Junlin Lan, Meiyue Li, Hao Wang, Fan Xie, Xiao Tian, Tianyue Gao, Junhua Chen, Zhenhong Yu, Melanie Schnell, Jens-Uwe Grabow, Qian Gou

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Abstract

This study presents the first integration of wavelet denoising with resonator-enhanced microwave spectroscopy to explore the formation and characteristics of gas-phase heterogeneous vinylene carbonate-(CO₂)_1–5 clusters. Through this innovative approach, faint spectral lines were detected with efficiency, enhancing our understanding of complex interaction patterns that govern the growth and stability of these molecular clusters. It was found that CO₂ aggregates preferentially around the vinylene carbonate molecule through C···O tetrel bonds at the carbonyl and ether groups, altering the typical self-aggregation topology of free CO₂ clusters. This leads to more symmetrical growth around the vinylene carbonate monomer. Our findings provide insights into the solvation mechanisms of compounds in supercritical CO₂ thereby advancing the understanding of subnanoscale CO₂ aggregation patterns.

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用小波增强微波光谱分析碳酸乙烯在CO2团簇生长和稳定性中的作用

本研究首次将小波去噪与谐振器增强微波光谱相结合，探讨了气相非均相碳酸乙烯-(CO2) 1-5簇的形成和特征。通过这种创新的方法，微弱的光谱线被有效地检测到，增强了我们对控制这些分子团簇生长和稳定性的复杂相互作用模式的理解。研究发现，CO2通过羰基和醚基上的C···O四键优先聚集在碳酸乙烯分子周围，改变了自由CO2团簇的典型自聚集拓扑结构。这使得碳酸乙烯单体周围的生长更加对称。我们的发现为化合物在超临界CO2中的溶剂化机制提供了见解，从而促进了对亚纳米级CO2聚集模式的理解。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.