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Wide-ranging Force Responsive Composites based on 1,2-dioxetane and ZnS as Luminescent Probes in Polyurethanes

Chinese Journal of Polymer Science 2023年第8期41卷 1162-1168,I0005页

作者： Jin-Hui Zhang Shuang Liu Yuan Yuan Yu-Lan Chen Department of Chemistry Tianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300354Chin State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012Chin

Combining the advantages of mechanochemiluminescence from 1,2-dioxetane and elastico-mechanoluminescence from ZnS particles,a new kind of mechanoluminescent polymer composites are *** can emit bright luminescence with two distinct colors at different strains,empowering a verstaile mechanochemical strategy for force sensing and damage detection at a wider force responsive range.

关键词： Mechanochemiluminescence 1,2-dioxetane Elastico-mechanoluminescence ZnS Polymer composites

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Nonadiabatic molecular dynamics on chemi-and bioluminescence of 1,2-dioxetane derivatives

Nonadiabatic molecular dynamics on chemi-and bioluminescence...

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第十三届全国量子化学会议

作者： Ling Yue Bo-wen Ding Ya-jun Liu Chao-yuan Zhu School of Science Xi'an J iaotong University College of Chemistry Beijing Normal University National Chiao Tung University Department of Applied Chemistry

Chemi-and bioluminescence, especially the ones from 1,2-dioxetane derivatives are widely applied in scientific analyses and commercial products. However, nonadiabatic molecular dynamics（NAMD） on the processes are challenges due to the biradical mechanism and nearly degenerated potential energy surface. To solve the problem, we developed several new approaches and improved the well-known NAMD software package Newton-X.1 By combining the spin-flip time-dependent density functional theory with Tully’s fewest switches on-the-fly trajectory surface hopping method, we simulated bioluminescent reaction of firefly and firefly squid. Not only did the dynamics simulation validate the gradually reversible charge transfer initiated luminescence（GRCTIL）mechanism we proposed previously, but also the theoretically estimated quantum yields of the singlet exci ted-state product fit the experimental values very well. To simulate the long-time neutral chemiluminescent processes of 1,2-dioxetanes which mainly provide triplet emitters through intersystem crossing, Zhu–Nakamura global switching algorithm2 was adopted and implemented into Newton-X package. The newly developed method does not require the calculation of nonadiabatic coupling vector so that can reduce the computational costs significantly. It was extensively compared with Tully’s local switching algorithm and showed excellent agreements with the later one and experimental measurements. The one-the-fly surface hopping simulation by the new algorithm and code provides a very close triplet quantum yields to the experimental value s,and affirms previously proposed biradical entropic trap mechanism.

关键词： Bioluminescence 1,2-dioxetane Surface hopping

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Multiple rapid-responsive probes for hypochlorite detection based on dioxetane luminophore derivatives

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Journal of Pharmaceutical Analysis 2022年第3期12卷 446-452页

作者： Yingai Sun Yuqi Gao Chunchao Tang Gaopan Dong Pei Zhao Dunquan Peng Tiantian Wang Lupei Du Minyong Li Department of Medicinal Chemistry Key Laboratory of Chemical Biology(MOE)School of PharmacyShandong UniversityJinan250012China School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou510006China State Key Laboratory of Microbial Technology Shandong UniversityJinan250100China

In recent years,various methods for detecting exogenous and endogenous hypochlorite have been studied,considering its essential role as a ***,the existing technologies still pose obstacles such as their invasiveness,high costs,and complicated *** the current study,we developed a glow-type chemiluminescent probe,hypochlorite chemiluminescence probe(HCCL)-1,based on the scaffold of Schaap's 1,2-dioxetane *** better explore the physiological and pathological functions of hypochlorite,we modified the luminophore scaffold of HCCL-1 to develop several probes,including HCCL-2,HCCL-3,and HCCL-4,which amplify the response signal of *** comparing the luminescent intensities of the four probes using the IVIS®system,we determined that HCCL-2 with a limit of detection of 0.166 mM has enhanced sensitivity and selectivity for tracking hypochlorite both in vitro and in vivo.

关键词： Glow-type Chemiluminescent probe 1,2-dioxetane Hypochlorite

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A specific and selective chemiluminescent probe for Pd^(2+) detection

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Chinese Chemical Letters 2019年第1期30卷 63-66页

作者： Yuqi Gao Yuxing Lin Tingting Liu Xiaomeng Zhang Feng Xu Pan Liu Lupei Du Minyong Li Department of Medicinal Chemistry Key Laboratory of Chemical Biology (MOE) School of Pharmacy Shandong University State Key Laboratory of Microbial Technology Shandong University

As an important transition metal catalyst, palladium is extensively used in many areas including electronics industry, petroleum industry, automobile industry and fine chemicals engineering. However,it brings harm to the environment as well as people's health. Herein, we managed to introduce a butynyl group to 1,2-dioxetane developing a reaction-based chemiluminescent probe as well as an imaging approach for monitoring palladium(II). Exhibiting enhanced total flux in Pd2+enriched areas, palladium chemiluminescent probe(PCL) may afford potential utility for detecting Pd2+in vitro, in cellulo and in vivo.

关键词： Chemiluminescent imaging Chemiluminescence 1,2-dioxetane Palladium(Ⅱ) Bioassays

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AMPPD及其对位异构体的化学发光解离机理的理论研究

AMPPD及其对位异构体的化学发光解离机理的理论研究

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中国化学会第28届学术年会

作者：岳岭刘亚军北京师范大学化学学院

3-（2’-spiroAdamantyl）-4-Methoxy-4-（m-Phosphoryloxy）-Phenyl-1,2-dioxetane（AMPPD）,在酶引发的脱磷酸化,然后解离生成激发态产物的反应,是应用于临床的化学发光免疫分析最成功的例子之一。我们在量子化学水平上,结合DFT与MS-CASPT2的方法,研究了AMPPD化学发光最关键的中间体3-（2’-spiroAdamantyl）-4-Methoxy-4-（m-hydroxyPhenyl）-1,2-dioxetane（AMPD）的热解离和发光过程。此外,为了揭示奇/偶选择规则的本质,我们也计算了AMPD对位异构体3-（2’-spiroAdamantyl）-4-Methoxy-4-（p-hydroxyPhenyl）-1,2-dioxetane（p-AMPD）。这是对AMPPD及其衍生物首次详细的理论研究。计算结果表明,AMPD解离经历了一个三过渡态,两中间体的电荷转移（CT）态的三步解离过程,通过此CT过程,反应物可以有效地生成激发态产物。而出乎意料的是,这一CT过程与通常认为的、由Adam等人1提出的CIEEL（chemically initiated electron exchange luminescence）机理并不相同,但却能与奇/偶选择规则吻合。这一差异暗示了我们必须重新并且深入考虑1,2-dioxetane及其衍生物在电荷转移引发的化学发光解离的机理。

关键词： AMPPD 1,2-dioxetane 化学发光

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