Progress in preparation and application of room temperature phosphorescencecarbon dots/SiO2 composites
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摘要: 碳点(Carbon dots,CDs)作为发光材料,在传感、信息安全、生物医学等领域具有重要应用潜力。然而,制备光学性能稳定、寿命长、发光效率高的CDs基室温磷光(RTP)材料仍然是一个巨大的挑战。将CDs固定在SiO2载体上构建CDs/SiO2复合材料,利用CDs与SiO2之间的协同作用,不仅可以提高CDs的分散性,实现CDs稳定的固态荧光;而且还能诱导三重激发态,产生稳定的三重态激子以实现CDs长寿命发光,这对拓展CDs基复合材料的应用领域具有重要意义。本文综述了近年来RTP CDs/SiO2复合材料的制备方法、性能与应用,总结了其发展中存在的问题,并对RTP CDs/SiO2复合材料的发展方向进行了展望。Abstract: Carbon dots (CDs) have great potential as luminescent materials in the fields of sensing, information security, biomedicine and so on. However, it is still a great challenge to prepare CDs based room temperature phosphorescence (RTP) materials with stable optical properties, long phosphorescence life and high quantum efficiency. Immobilizing CDs on SiO2 matrix to construct the CDs/SiO2 composites, which can utilize the synergy between CDs and SiO2. It not only can improve the dispersion of CDs to achieve stable solid-state fluorescence of CDs, but also can generate stable triplet excitons to achieve long-life phosphorescence of CDs. The RTP CDs/SiO2 composite is of great significance for expanding the phosphorescent application field of CDs-based composites. In this paper, the preparation methods, properties and applications of phosphorescent CDs/SiO2 composites in recent years were reviewed. The existing problems in the development of phosphorescent CDs/SiO2 composites were summarized, and the development direction of CDs/SiO2 composites was prospected.
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图 1 碳点(CDs)的荧光、延迟荧光、磷光及室温磷光产生示意图
S0—Ground state; S1—Single excited state; Sn—High-level singlet excited state; Abs—Absorption; IC—Internal conversion; FL—Fluorescence; TADF—Delay fluorescence; EC—External conversion; ISC—Intersystem crossing; RISC—Reverse intersystem crossing; Phos.—Phosphorescence; RTP—Room temperature phosphorescence; Tn—High-energy triplet excited states; T1—High-level singlet excited state; T1*— High-level singlet excited state (new)
Figure 1. Fluorescence, delayed fluorescence, phosphorescence androom-temperature phosphorescence generation schematicof carbon dots (CDs)
图 3 (a) 磷光碳点(PCDs)和体系1~4的制备过程示意图;(b)在365 nm光照射下体系1~4的水相荧光和余辉图像;(c)体系4在水环境中可能的余辉机制[42]
Rh6G—Rodamine 6G; RhB—Rodamine B; SR101—Sulforhodamine 101; Exc.—Excitation; Fluo.—Fluorescence; ET—Energy transfer
Figure 3. (a) Schematic diagram of the preparation process of phosphorescent carbon points (PCDs) and system 1-4; (b) Aqueous fluorescence and afterglow images of system 1-4 under 365 nm light irradiation; (c) Possible afterglow mechanism of system 4 in aqueous environment[42]
图 5 彩色磷光CDs/SiO2复合材料[47](a)和GCDs/SiO2-OCDs复合材料[48 ](b)的制备示意图
o-PD—o-phenylenediamine; BCDs/SiO2—Blue phosphoresence CDs/SiO2; RCDs/SiO2—Red phosphoresence CDs/SiO2; GCDs/SiO2—Green phosphoresence CDs/SiO2; YCDs/SiO2—Yellow phosphoresence CDs/SiO2; FRET—Fluorescence resonance energy transfer; R—Interparticle distance; OCDs—Orange CDs
Figure 5. Schematic diagrams for the preparations of colorful phosphorescent CDs/SiO2 composites[47] (a) and GCDs/SiO2-OCDs composites[48] (b)
图 10 (a) CDs-RhB/SiO2在活体小鼠体内原位活化和余辉检测示意图;(b)时间门控生物成像的实例说明;(c)不同浓度CDs-RhB/SiO2皮下植入小鼠体内荧光和磷光图像;(d)不同浓度CDs-RhB/SiO2在体内的荧光和余辉强度[43]
CCD—Charge coupled device; RhB—Rhodamine B
Figure 10. (a) Schematic illustration of in situ activation and detection of afterglow of the CDs-RhB/SiO2 in living mice; (b) Illustration of time-gated bioimaging; (c) In vivo fluorescence and phosphorescence images of mice with the subcutaneous implantation of different concentration of CDs-RhB/SiO2; (d) Fluorescence and afterglow intensities of CDs-RhB/SiO2 in vivo with different concentrations[43]
图 12 (a)基于安全油墨的时分双工示意图;(b)基于时分双工技术的时空重叠(I、II)和时空分离(III、IV)模式[74];(c)基于安全油墨的信息加密原理图[54]
Figure 12. (a) Time division duplex diagram based on safety ink; (b) Space-time overlap (I, II) and space-time separation (III, IV) modes based on time division duplex technology[74]; (c) Schematic diagram of information encryption based on security ink[54]
图 13 在365 nm紫外光照射下用RTP CDs/SiO2粉末在塑料片上显影(a)和关闭紫外灯指纹图像上的具体细节(b)[78];(c) RTP CDs/SiO2粉末的橙色余辉指纹显影[48]
Figure 13. Images of a fresh fingerprint developed by RTP CDs/SiO2 powder on the plastic sheet under 365 nm UV light on (a) and off (b) with some specific details [78]; (c) Orange afterglow fingerprint development of RTP CDs/SiO2 powder[48]
表 1 典型一步法合成RTP CDs/SiO2复合材料性能参数
Table 1. Typical performance parameters of RTP CDs/SiO2 composites synthesized by typical one-step method
Sample Materials Method RTP Em/nm Lifetime/s RTP QY/% Ref. CPDs/SNSs TEOS Hydrothermal 520 1.86 11.6 [35] N-CDs/SiO2 TEOS, triethylenetetramine Hydrothermal 510 1.81 6 [36] CPDs/SiO2 TEOS, EDA Hydrothermal 440 1.26 — [37] CDs/SiO2 APTES Hydrothermal 430 0.81 10.34 [38] CPDs/SiO2 AEAPMS, phosphoric acid Microwave-assisted hydrothermal 515 1.32 11.42 [39] CDs/SiO2 Glucose, chitosan, PVP, CA, APTES Muffle furnace 525 0.38 1.3 [40] Notes: CPDs—Carbonized polymer point; N-CDs—Nitrogen doped carbon dots; SNSs—Silica nanospheres; TEOS—Tetraethoxysilane; EDA—Ethanediamine; APTES—3-aminopropyl triethoxysilane; AEAPMS—3-(2-aminoethyl amino)propyl dimethoxy-methylsilane; PVP—Polyvinylpyrrolidone; CA—Citric acid; Em—Emission; RTP QY—Room temperature phosphorescence quantum yield. 表 2 典型RTP CDs/SiO2复合材料性能参数
Table 2. Typical RTP CDs/SiO2 composite material performance parameters
Materials RTP Em/nm ΔEST/eV Lifetime/s RTP QY/% Ref. Alkali lignin 520 0.300 0.834 5.97 [50] Rice husk 464 0.155 5.720 26.35 [51] Urea, APTES 462 0.103 2.030 50.17 [61] EDA, phosphoric acid, TEOS 505 0.380 2.190 7.40 [63] TM-40 colloidal silica, terephthalic acid 424 — 0.237 1.47 [64] CA, TEOS, benzidine monohydrochloride 444 0.320 1.110 — [65] Ethanolamine, TEOS, phosphoric acid 510 — 0.847 12.10 [66] Notes: ΔEST—Energy gap between S1 and Tn; TM-40—Tipes of colloidal silica; CA—Citric acid. -
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