Mechanistic investigation of a visible light mediated dehalogenation/cyclisation reaction using iron(iii), iridium(iii) and ruthenium(ii) photosensitizers

Aydogan Akin; Bangle Rachel E.; De Kreijger SimonDickenson John C.Singleton Michael L.Cauet EmilieCadranel AlejandroMeyer Gerald J.Elias BenjaminSampaio Renato N.Troian-Gautier Ludovic

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Mechanistic investigation of a visible light mediated dehalogenation/cyclisation reaction using iron(iii), iridium(iii) and ruthenium(ii) photosensitizers

机译：机械的可见光的调查脱卤作用/ cyclisation反应介导的使用铁(iii),铱(iii)和钌(ii)敏化

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The mechanism of a visible light-driven dehalogenation/cyclization reaction was investigated using ruthenium(ii), iridium(iii) and iron(iii) photosensitizers by means of steady-state photoluminescence, time-resolved infrared spectroscopy, and nanosecond/femtosecond transient absorption spectroscopy. The nature of the photosensitizer was found to influence the product distribution such that the dehalogenated, non-cyclized products were only detected for the iron photosensitizer. Strikingly, with the iron photosensitizer, large catalytic yields required a low dielectric solvent such as dichloromethane, consistent with a previous publication. This low dielectric solvent allowed ultrafast charge-separation to outcompete geminate charge recombination and improved cage escape efficiency. Further, the identification of reaction mechanisms unique to the iron, ruthenium, and iridium photosensitizer represents progress towards the long-sought goal of utilizing earth-abundant, first-row transition metals for emerging energy and environmental applications.

机译：可见light-driven机制脱卤作用/环化反应调查使用钌(ii)、铱(iii)和铁(iii)敏化的稳态光致发光,时间分辨红外光谱和纳秒/飞秒瞬态吸收光谱。光敏剂被发现影响dehalogenated等产品销售,non-cyclized产品只检测到的铁光敏剂。光敏剂,大型催化收益率要求低介电溶剂如二氯甲烷、符合之前的出版物。电介质溶剂允许超快电荷分离战胜成双的费用重组和改进的笼子里逃脱效率。反应机制的铁,钌、铱光敏剂代表的长期目标的进展利用地球上充足,板凳过渡金属对新兴能源和环境应用程序。

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《Catalysis science & technology》 |2021年第24期|8037-8051|共15页
作者
Aydogan Akin; Bangle Rachel E.; De Kreijger SimonDickenson John C.Singleton Michael L.Cauet EmilieCadranel AlejandroMeyer Gerald J.Elias BenjaminSampaio Renato N.Troian-Gautier Ludovic;
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作者单位

Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA;

Univ Catholique Louvain UCLouvain, Inst Matiere Condensee & Nanosci IMCN, Mol Chem Mat & Catalysis MOST, Pl Louis Pasteur 1,Bte L4-01-02, B-1348 Louvain La Neuve, Belgium;

Friedrich Alexander Univ Erlangen Nurnberg, Interdisciplinary Ctr Mol Mat ICMM, Dept Chem & Pharm, Egerlandstr 3, D-91058 Erlangen, GermanyUniv Libre Bruxelles, Spect Quantum Chem & Atmospher Remote Sensing CP, 50 Av FD Roosevelt, B-1050 Brussels, Belgium;

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正文语种英语
中图分类汉语教学;
关键词
Iron; Photosensitizing Agents; transition metalPhotosensitizersReaction MechanismsVisible LightCHARGE RECOMBINATIONENVIRONMENTAL APPLICATION;

机译：铁;Photosensitizing代理;过渡metalPhotosensitizersReaction MechanismsVisibleLightCHARGE RECOMBINATIONENVIRONMENTAL应用程序;

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Mechanistic investigation of a visible light mediated dehalogenation/cyclisation reaction using iron(iii), iridium(iii) and ruthenium(ii) photosensitizers

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