One-Pot Synthesis of Acetylacetonate-Based Isomeric Phosphorescent Cyclometalated Iridium(III) Complexes via Random Cyclometalation: A Strategy for Excited-State Manipulation,Inorganic Chemistry

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One-Pot Synthesis of Acetylacetonate-Based Isomeric Phosphorescent Cyclometalated Iridium(III) Complexes via Random Cyclometalation: A Strategy for Excited-State Manipulation
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-01-09 , DOI: 10.1021/acs.inorgchem.2c03597
Peng Tao _{1,

2,

3} , Zhuang Lv ₄ , Fang-Qing Zhao ₁ , Xiao-Kang Zheng _{1,

2} , He Jiang ₂ , Wentao Li ₂ , Yongjing Deng ₁ , Shujuan Liu ₁ , Guohua Xie ₅ , Wai-Yeung Wong _{2,

3} , Qiang Zhao ₁

Affiliation

The excited-state manipulation of the phosphorescent iridium(III) complexes plays a vital role in their photofunctional applications. The development of the molecular design strategy promotes the creative findings of novel iridium(III) complexes. The current molecular design strategies for iridium(III) complexes mainly depend on the selective cyclometalation of the ligands with the iridium(III) ion, which is governed by the steric hindrance of the ligand during the cyclometalation. Herein, a new molecular design strategy (i.e., random cyclometalation strategy) is proposed for the effective excited-state manipulation of phosphorescent cyclometalated iridium(III) complexes. Two series of new and separable methoxyl-functionalized isomeric iridium(III) complexes are accessed by a one-pot synthesis via random cyclometalation, resulting in a dramatic tuning of the phosphorescence peak wavelength (∼57 nm) and electrochemical properties attributed to the high sensitivity of their excited states to the position of the methoxyl group. These iridium(III) complexes show intense phosphorescence ranging from the yellow (567 nm) to the deep-red (634 nm) color with high photoluminescence quantum yields of up to 0.99. Two deep-red emissive iridium(III) complexes with short decay lifetimes are further utilized as triplet emitters to afford efficient solution-processed electroluminescence with reduced efficiency roll-offs.

中文翻译：

通过随机环金属化一锅法合成基于乙酰丙酮的异构磷光环金属化铱 (III) 配合物：一种激发态操纵策略

磷光铱 (III) 配合物的激发态操作在其光功能应用中起着至关重要的作用。分子设计策略的发展促进了新型铱（III）配合物的创造性发现。目前铱 (III) 配合物的分子设计策略主要取决于配体与铱 (III) 离子的选择性环金属化，其受环金属化过程中配体的空间位阻控制。在此，提出了一种新的分子设计策略（即随机环金属化策略），用于有效控制磷光环金属化铱 (III) 配合物的激发态。两个系列的新的和可分离的甲氧基功能化异构铱 (III) 配合物通过随机环金属化一锅合成获得，导致磷光峰值波长（~57 nm）和电化学性质的显着调整，这归因于它们的激发态对甲氧基位置的高度敏感性。这些铱 (III) 配合物显示出从黄色 (567 nm) 到深红色 (634 nm) 的强烈磷光，具有高达 0.99 的高光致发光量子产率。两种具有短衰变寿命的深红色发光铱 (III) 配合物被进一步用作三线态发射体，以提供高效的溶液处理电致发光，同时降低效率滚降。这些铱 (III) 配合物显示出从黄色 (567 nm) 到深红色 (634 nm) 的强烈磷光，具有高达 0.99 的高光致发光量子产率。两种具有短衰变寿命的深红色发光铱 (III) 配合物被进一步用作三线态发射体，以提供高效的溶液处理电致发光，同时降低效率滚降。这些铱 (III) 配合物显示出从黄色 (567 nm) 到深红色 (634 nm) 的强烈磷光，具有高达 0.99 的高光致发光量子产率。两种具有短衰变寿命的深红色发光铱 (III) 配合物被进一步用作三线态发射体，以提供高效的溶液处理电致发光，同时降低效率滚降。

更新日期：2023-01-09

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