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121.
Shuangqi Pi Quansong Li Ling Yue Prof. Dr. Ya-Jun Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(18):5712-5720
A first-generation pair of chemiluminescent formaldehyde (FA) probes (CFAP540 and CFAP700) was reported recently. CFAP540 and CFAP700, with high selectivity and sensitivity to FA, are, respectively, suitable in cell and in vivo. Experimentalists have confirmed that both probes utilize a general 2-aza-Cope FA-reactive trigger and a chemiluminogenic phenoxydioxetane scaffold. The mechanism and detailed process of CFAP chemiluminescence (CL) remain largely unknown. In the present paper, (time-dependent) density functional theory calculations are performed on the entire reaction process of CFAP540 with FA to produce CL. The calculations elucidated the CL-producing process: FA initiates the decomposition of CFAP540 by dehydration condensation, and a phenoxy 1,2-dioxetane is formed through a series of reactions of aza-Cope rearrangement, hydrolysis of imine, and β-elimination of alkoxyl group. Afterwards, the produced phenoxy 1,2-dioxetane decomposes to produce the m-oxybenzoate derivative in the first singlet state (S1) via two crossings between potential energy surfaces of the ground state (S0) and S1 state. This m-oxybenzoate derivative was assigned as the light emitter of the CFAP540 CL. The CL-producing process and assignment of the light emitter of CFAP700 CL are similar with the corresponding ones of CFAP540. By analyzing the D-π-A architecture of the light emitters of CFAP540 and CFAP700, a series of CFAPs is theoretically designed and a scheme to modulate their CL from visible to near-infrared region is proposed by adjusting the length and structure of the π-bridge. 相似文献
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Inmaculada Robina Silvia Gómez-Bujedo José G. Fernández-Bolaños José Fuentes 《合成通讯》2013,43(13):2379-2397
To prepare C-sulfonate derivatives of disaccharides two different strategies were followed. Thus 6- and 6′-C-sulfocellobiosides 4 and 10–12 were prepared starting from a suitably protected cellobioside. The 6′-C-sulfoaminocellobioside 18 was prepared by construction of the molecule through a glycosylation reaction. In both cases, the synthetic pathway involves regioselective tosylation, introduction of a sulfur atom by nucleophilic displacement with potassium thioacetate and oxidation with hydrogen peroxide. 相似文献
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Gangxian Zhu Dichen Li Anfeng Zhang Gang Pi Yiping Tang 《Optics & Laser Technology》2012,44(2):349-356
To investigate the influencing rules of the variations of powder and laser defocusing distance on surface quality and obtain the smooth surface of parts in laser direct metal deposition, the thin-walled metal parts were fabricated under three different powder defocusing distances and three different laser defocusing distances conditions. The experimental results show that a high surface quality can be obtained with the powder focussed below the substrate and laser focussed above the substrate process, and the variation in which the powder focus moves from above to below the melt pool plays a leading role and the variation in which the laser focus moves from above to below the melt pool plays a supplementary role in the influence on the surface quality. To explain the experimental results, a simple model of the track height is established. 相似文献
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Daniel Roca‐Sanjuán Marcus Lundberg David A. Mazziotti Roland Lindh 《Journal of computational chemistry》2012,33(26):2124-2126
In the preceding paper results are presented, which are in serious conflict with state‐of‐the‐art ab initio method. Based on these new results the authors propose a new explanation of the reason for the preferential production of a phosphorescent state. Here we show that these controversial results are flawed, since the model use exclude biradical electron structures. © 2012 Wiley Periodicals, Inc. 相似文献