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在具有空前固态量子产率和稳定性的层状主体基质中受限合成碳氮化物。

Confined Synthesis of Carbon Nitride in a Layered Host Matrix with Unprecedented Solid-State Quantum Yield and Stability.

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.

出版信息

Adv Mater. 2018 Jan;30(2). doi: 10.1002/adma.201704376. Epub 2017 Nov 27.

Abstract

Fluorescent carbon nanomaterials have drawn tremendous attention for their intriguing optical performances, but their employment in solid-state luminescent devices is rather limited as a result of aggregation-induced photoluminescence quenching. Herein, ultrathin carbon nitride (CN) is synthesized within the 2D confined region of layered double hydroxide (LDH) via triggering the interlayer condensation reaction of citric acid and urea. The resulting CN/LDH phosphor emits strong cyan light under UV-light irradiation with an absolute solid-state quantum yield (SSQY) of 95.9 ± 2.2%, which is, to the best of our knowledge, the highest value of carbon-based fluorescent materials ever reported. Furthermore, it exhibits a strong luminescence stability toward temperature, environmental pH, and photocorrosion. Both experimental studies and theoretical calculations reveal that the host-guest interactions between the rigid LDH matrix and interlayer carbon nitride give the predominant contribution to the unprecedented SSQY and stability. In addition, prospective applications of the CN/LDH material are demonstrated in both white light-emitting diodes and upconversion fluorescence imaging of cancer cells.

摘要

荧光碳纳米材料因其有趣的光学性能而引起了极大的关注,但由于聚集诱导的光致荧光猝灭,它们在固态发光器件中的应用相当有限。在此,通过触发柠檬酸和尿素的层间缩合反应,在层状双氢氧化物(LDH)的 2D 限制区域内合成了超薄的碳氮化物(CN)。所得的 CN/LDH 荧光粉在紫外光照射下发出强烈的蓝光,其绝对固态量子产率(SSQY)为 95.9±2.2%,据我们所知,这是迄今为止报道的碳基荧光材料的最高值。此外,它还表现出对温度、环境 pH 值和光腐蚀的强发光稳定性。实验研究和理论计算都表明,刚性 LDH 基质与层间碳氮化物之间的主客体相互作用是产生前所未有的 SSQY 和稳定性的主要原因。此外,CN/LDH 材料在白光发光二极管和癌细胞的上转换荧光成像中的潜在应用也得到了证明。

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