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排序方式: 共有233条查询结果,搜索用时 140 毫秒
231.
Dr. Jiawen Fang Prof. Dr. Yiou Wang Mariam Kurashvili Dr. Sebastian Rieger Dr. Wiktor Kasprzyk Qingli Wang Prof. Dr. Jacek K. Stolarczyk Prof. Dr. Jochen Feldmann Dr. Tushar Debnath 《Angewandte Chemie (International ed. in English)》2023,62(33):e202305817
Photocatalytic water splitting is a promising approach to generating sustainable hydrogen. However, the transport of photoelectrons to the catalyst sites, usually within ps-to-ns timescales, is much faster than proton delivery (∼μs), which limits the activity. Therefore, the acceleration of abstraction of protons from water molecules towards the catalytic sites to keep up with the electron transfer rate can significantly promote hydrogen production. The photobasic effect that is the increase in proton affinity upon excitation offers means to achieve this objective. Herein, we design photobasic carbon dots and identify that internal pyridinic N sites are intrinsically photobasic. This is supported by steady-state and ultrafast spectroscopic measurements that demonstrate proton abstraction within a few picoseconds of excitation. Furthermore, we show that in water, they form a unique four-level lasing scheme with optical gain and stimulated emission. The latter competes with photocatalysis, revealing a rather unique mechanism for efficiency loss, such that the stimulated emission can act as a toggle for photocatalytic activity. This provides additional means of controlling the photocatalytic process and helps the rational design of photocatalytic materials. 相似文献
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233.
Youxin Fu Jun.-Prof. Dr. Nadja A. Simeth Dr. Ryojun Toyoda Dr. Robert Brilmayer Prof. Dr. Wiktor Szymanski Prof. Dr. Ben L. Feringa 《Angewandte Chemie (International ed. in English)》2023,62(16):e202218203
Light-induced 9,10-phenanthrenequinone-electron-rich alkene ( PQ-ERA ) photocycloadditions are an attractive new type of photoclick reaction, featuring fast conversions and high biocompatibility. However, the tunability of the reaction was hardly investigated up to now. To this end, we explored the influence of substituents on both reaction partners and the reaction rate between the PQs and ERAs . We identified new handles for functionalization and discovered that using enamines as ERAs leads to drastically enhanced rates (>5400 times faster), high photoreaction quantum yields ( ΦP , up to 65 %), and multicolor emission output as well as a high fluorescence quantum yield of the adducts ( ΦF , up to 97 %). Further investigation of the photophysical and photochemical properties provided insights to design orthogonal reaction systems both in solution and on nanoparticle surfaces for ultrafast chemoselective functionalization by photoclick reactions. 相似文献