Barbituric acid derivative supramolecular assembly as a matrix for oxygen-sensitive photodriven formation of superoxide and carbon-centered radicals

IF 3.1 3区 化学 Q3 CHEMISTRY, PHYSICAL Chemical Physics Letters Pub Date : 2025-02-28 DOI:10.1016/j.cplett.2025.141957
Alexandra A. Timralieva , Natalia A. Chumakova , Alexander V. Fionov , Elizaveta A. Konstantinova , Ruslan B. Zaripov , Maxim A. Demekhin , Maxim E. Radchenko , Alexander S. Novikov , Sergey O. Travin , Alexander I. Kokorin , Ekaterina V. Skorb
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Abstract

Supramolecular system of native barbituric acid and its 1,3-dimethyl derivative with melamine was studied using continuous-wave Q-band EPR spectroscopy. For separation of EPR signals, a special mathematical method was developed and applied. One axial symmetry signal and three singlet signals were detected and interpreted as belonging to superoxide radical and C-centered radicals, correspondingly. Radical activity of the system and predominance of specific radical centers were found to depend on compounds ratio, pH and light irradiation as well as samples storage time and oxygen presence. Quantum chemical calculations were performed to propose the localization of C-centered radicals in both supramolecular systems.

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巴比妥酸衍生物超分子组装作为氧敏光驱动形成超氧化物和碳中心自由基的基质
采用连续q波段EPR光谱法研究了天然巴比妥酸及其1,3-二甲基三聚氰胺衍生物的超分子体系。为了实现EPR信号的分离,提出了一种特殊的数学方法。检测到一个轴对称信号和三个单线态信号,分别属于超氧自由基和c中心自由基。发现体系的自由基活性和特定自由基中心的优势取决于化合物的配比、pH、光照以及样品的储存时间和氧的存在。量子化学计算提出了c中心自由基在两种超分子体系中的定位。
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来源期刊
Chemical Physics Letters
Chemical Physics Letters 化学-物理:原子、分子和化学物理
CiteScore
5.70
自引率
3.60%
发文量
798
审稿时长
33 days
期刊介绍: Chemical Physics Letters has an open access mirror journal, Chemical Physics Letters: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Chemical Physics Letters publishes brief reports on molecules, interfaces, condensed phases, nanomaterials and nanostructures, polymers, biomolecular systems, and energy conversion and storage. Criteria for publication are quality, urgency and impact. Further, experimental results reported in the journal have direct relevance for theory, and theoretical developments or non-routine computations relate directly to experiment. Manuscripts must satisfy these criteria and should not be minor extensions of previous work.
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