A Thermally Populated Germylene-Based Donor-Acceptor Diradical.

IF 19.3 1区 材料科学 Q1 CHEMISTRY, PHYSICAL ACS Energy Letters Pub Date : 2024-08-27 DOI:10.1002/anie.202411180
Yu Zhao, Yuchen Zhang, Tao Wang, Runbo Pei, Yue Zhao, Xiao-Song Xue, Xinping Wang
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Abstract

This work reports synthesis of a germylene based donor-acceptor molecule and its thermal excitation to a triplet state by coordination with a Lewis acid. Products have been characterized by single crystal X-ray diffraction, EPR spectroscopy, and SQUID measurement, in conjunction with DFT calculation. The singlet-triplet energy gap of the donor-acceptor molecule is dramatically reduced from -18.8 to -7.2 kcal/mol by the coordination with B(C6F5)3 (BCF), which enables an intramolecular single electron transfer from one germylene moiety to another upon heating, forming an intramolecular radical ion pair with diradical character. The work provides an approach to the formation of thermally populated open-shell species of heavier main group elements.

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一种基于热填充胚芽烯的供体-受体二拉基。
这项研究报告了一种基于锗烯的供体-受体分子的合成及其通过与路易斯酸配位而热激发到三重态的过程。通过单晶 X 射线衍射、EPR 光谱和 SQUID 测量以及 DFT 计算,对产品进行了表征。通过与 B(C6F5)3 (BCF)配位,供体-受体分子的单重态-三重态能隙从-18.8 kcal/mol 显著降低到-7.2 kcal/mol,从而在加热时实现了分子内单电子从一个亚甲二氧基转移到另一个亚甲二氧基,形成了具有二叉性质的分子内自由基离子对。这项工作为形成较重主族元素的热填充开壳物种提供了一种方法。
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来源期刊
ACS Energy Letters
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍: ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.
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