Water-driven Photoluminescence Reversibility in CdSe/CdS Quantum Dots Polymer Composite

Jun-hu CAI; Chen-hui WANG; Xin-pei HU; En-guo CHEN; Sheng XU; Yun YE; Tai-liang GUO

doi:10.37188/CJL.20210401

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Water-driven Photoluminescence Reversibility in CdSe/CdS Quantum Dots Polymer Composite

Synthesis and Properties of Materials | Updated：2022-05-23

- Water-driven Photoluminescence Reversibility in CdSe/CdS Quantum Dots Polymer Composite Enhanced Publication
- Chinese Journal of Luminescence Vol.43, Issue 5, (2022)
- Affiliations：
  
  National-Local United Engineering Laboratory of Flat Panel Display Technology, College of Physics and Information Engineering, Fuzhou University,Fuzhou,China,350108;Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China (Mindu Innovation Laboratory),Fuzhou,China,350108
- Author bio：
- Funds：
  
  National Natural Science Foundation of China(62175032);Fujian Provincial Natural Science Foundation Project(2021J01579);Fujian Provincial key science and technology Project(2021HZ021001);Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China(2020ZZ111)
- DOI：10.37188/CJL.20210401 CLC： O482.31
- Published：2022-05，
  
  Received：28 December 2021，
  
  Revised：15 January 2022，
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Cite this article
Jun-hu CAI, Chen-hui WANG, Xin-pei HU, et al. Water-driven Photoluminescence Reversibility in CdSe/CdS Quantum Dots Polymer Composite. [J]. Chinese Journal of Luminescence 43(5):714-724(2022)
DOI：

Jun-hu CAI, Chen-hui WANG, Xin-pei HU, et al. Water-driven Photoluminescence Reversibility in CdSe/CdS Quantum Dots Polymer Composite. [J]. Chinese Journal of Luminescence 43(5):714-724(2022) DOI： 10.37188/CJL.20210401.

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"对量子点表面缺陷的有效钝化，使得量子点的晶胞更趋于理想化。进一步通过实验发现，当复合材料从水中取出干燥后，由于量子点表面缺陷态又重新暴露，光致发光强度和荧光量子产率又恢复到初始值。受所发现的荧光可逆现象的启发，本文基于CdSe/CdS@PDMS-PUa复合材料提出了一种具有荧光响应的液体高度传感器，通过荧光亮度的变化可以判断容器内液体的高度值。这些发现不仅揭示了CdSe/CdS量子点水致荧光可逆特性，同时拓宽了量子点聚合物复合材料在光电领域的应用，具有重要的科学意义和应用前景。" } ] } ] }, { "lang": "en", "data": [ { "name": "p", "data": [ { "name": "text", "data": "Quantum dots are a promising star material in the field of new optoelectronic devices due to their excellent optical and electrical properties. In this work, we prepare the CdSe/CdS@PDMS-PUa composite by encapsulating core/shell CdSe/CdS quantum dots into an amino-terminated polydimethylsiloxane(PDMS-PUa) polymer matrix, which shows water-driven enhanced photoluminescence(PL) intensity and photoluminescence quantum yield(PLQY). After the analysis of fluorescent decay curve and diffuse reflectance spectrum, the reason for this enhancement is found to be the passivation of the surface defects of the quantum dots by H" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "O" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": " and OH" }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] }, { "name": "text", "data": " in water, making the unit cell of the quantum dots more idealized. However, when the composite is taken out of the water for drying, the defect states are exposed again, and both PL and PLQY return to their original values. Inspired by the water-driven PL reversibility in CdSe/CdS@PDMS-PUa composite, a liquid height sensor with fluorescence response is proposed based on the CdSe/CdS@PDMS-PUa composite, which can judge the liquid height value in the container through the change of fluorescence intensity. These findings not only reveal the reversible characteristics of CdSe/CdS quantum dots, but also broaden the application of quantum dots polymer composites in the field of optoelectronics, which has important scientific significance and application prospects." } ] } ] } ], "keyword": [ { "lang": "zh", "data": [ [ { "name": "text", "data": "CdSe/CdS量子点" } ], [ { "name": "text", "data": "水" } ], [ { "name": "text", "data": "荧光可逆" } ], [ { "name": "text", "data": "缺陷钝化" } ], [ { "name": "text", "data": "传感" } ] ] }, { "lang": "en", "data": [ [ { "name": "text", "data": "CdSe/CdS quantum dots" } ], [ { "name": "text", "data": "polymer" } ], [ { "name": "text", "data": "water" } ], [ { "name": "text", "data": "photoluminescence reversibility" } ], [ { "name": "text", "data": "sensing" } ] ] } ], "highlights": [], "body": [ { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "1" } ], "title": [ { "name": "text", "data": "引言" } ], "level": "1", "id": "s1" } }, { "name": "p", "data": [ { "name": "text", "data": "近年来，镉系量子点以其独特的光电特性，在光电领域得到了迅速的发展。其色纯度高、发光颜色可调和荧光量子产率高等光学性能使得其在平板显示和照明等领域受到了广泛的关注" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "1", "type": "bibr", "rid": "R1", "data": [ { "name": "text", "data": "1" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "7", "type": "bibr", "rid": "R7", "data": [ { "name": "text", "data": "7" } ] } } ], "rid": [ "R1", "R2", "R3", "R4", "R5", "R6", "R7" ], "text": "1-7", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。在光伏领域应用方面，其带隙易调控、电荷迁移率、在可见光范围有比较好的吸光性能等优势也使其大有用武之地" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "8", "type": "bibr", "rid": "R8", "data": [ { "name": "text", "data": "8" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "14", "type": "bibr", "rid": "R14", "data": [ { "name": "text", "data": "14" } ] } } ], "rid": [ "R8", "R9", "R10", "R11", "R12", "R13", "R14" ], "text": "8-14", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。与此同时，较宽的增益谱、较低的成本以及作为可饱和吸收镜的关键材料使其在激光领域也具有非常大的潜力" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "15", "type": "bibr", "rid": "R15", "data": [ { "name": "text", "data": "15" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "16", "type": "bibr", "rid": "R16", "data": [ { "name": "text", "data": "16" } ] } } ], "rid": [ "R15", "R16" ], "text": "15-16", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。此外，量子点具有颜色多样、荧光强度强、灵敏度高、容易进行界面修饰连接、生物相容性好等优点，在基因定位、蛋白检测、生物成像、肿瘤治疗方面也有着广阔的应用前景" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "17", "type": "bibr", "rid": "R17", "data": [ { "name": "text", "data": "17" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "19", "type": "bibr", "rid": "R19", "data": [ { "name": "text", "data": "19" } ] } } ], "rid": [ "R17", "R18", "R19" ], "text": "17-19", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "近年来，基于镉系量子点所开展的荧光传感器研究也越来越多" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "20", "type": "bibr", "rid": "R20", "data": [ { "name": "text", "data": "20" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "23", "type": "bibr", "rid": "R23", "data": [ { "name": "text", "data": "23" } ] } } ], "rid": [ "R20", "R21", "R22", "R23" ], "text": "20-23", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。一方面，镉系量子点的带隙、纳米结构、表面积与体积比、电导率和热导率以及迁移率等一系列物理和化学特性会随着不同的环境条件而变化，这使得量子点材料成为传感应用的理想选择" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "24", "type": "bibr", "rid": "R24", "data": [ { "name": "text", "data": "24" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。另一方面，光学传感器与其他类型传感器相比具有许多优势，因为人眼对亮度变化具有极高的敏感性，范围可以从10" }, { "name": "sup", "data": [ { "name": "text", "data": "-6" } ] }, { "name": "text", "data": "~10" }, { "name": "sup", "data": [ { "name": "text", "data": "6" } ] }, { "name": "text", "data": " cd·m" }, { "name": "sup", "data": [ { "name": "text", "data": "-2" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "[25]" } ] }, { "name": "text", "data": "。例如，Potyrailo等利用镉系量子点可逆且可调的晶格尺寸，开发了一种荧光响应的气体传感器" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "26", "type": "bibr", "rid": "R26", "data": [ { "name": "text", "data": "26" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。Muhammad等利用CdSe量子点(CdSe QDs)对环境响应的表面积，制备了Ag/F8-CdSe QDs/Ag多用途荧光响应传感器" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而，基于镉系量子点在液体传感方面的研究还是比较欠缺。因为该类纳米晶本身可以通过水分降解，容易造成荧光不可逆的降解猝灭，大大限制了其在液体传感方面的应用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了开发镉系量子点在液体传感器上的应用，首先应要解决的是量子点对水的不可逆降解猝灭，然后再寻找该材料能够对环境产生荧光响应的调制机制。核壳结构的镉系量子点可以有效地降低核层外的面缺陷，从而提高发光效率和光学稳定性。相比CdSe/ZnS量子点核壳结构，CdSe/CdS量子点核壳晶格有着优异的匹配度，界面缺陷少" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "28", "type": "bibr", "rid": "R28", "data": [ { "name": "text", "data": "28" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。基于此，本文通过将核壳CdSe/CdS量子点封装到氨基封端的聚二甲基硅氧烷(PDMS-PUa)聚合物基质中制备CdSe/CdS@PDMS-PUa复合材料，并探索其水致荧光可逆现象，进一步基于该量子点聚合物复合材料开发了一种具有荧光响应的液体传感器，拓宽了镉系量子点复合材料在光电领域的应用。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2" } ], "title": [ { "name": "text", "data": "实验" } ], "level": "1", "id": "s2" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2.1" } ], "title": [ { "name": "text", "data": "样品制备" } ], "level": "2", "id": "s2a" } }, { "name": "p", "data": [ { "name": "text", "data": "本实验所使用的量子点材料为核壳结构的镉系量子点，核为CdSe，壳为CdS，购自广东普加福光电科技有限公司。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "PDMS-PUa聚合物的合成：在氮气下将NH" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "-PDMS-NH" }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "(2.5 mL)、甲苯(5 mL)和甲苯二异氰酸酯(0.17 g)加入到三颈烧瓶中。然后将混合物在23 ℃的温度下通过强力磁力搅拌处理24 h。最后将所得粘性溶液储存直至进一步使用。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "CdSe/CdS@PDMS-PUa复合材料的合成：将核壳CdSe/CdS量子点与PDMS-PUa共聚物溶液混合搅拌30 min，得到均匀的粘稠溶液。然后将所得溶液倒入临时特氟龙模具上并置于真空干燥箱中以蒸发溶剂，直至形成复合凝胶。最后，将复合材料剥离以供进一步使用。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "2.2" } ], "title": [ { "name": "text", "data": "样品表征" } ], "level": "2", "id": "s2b" } }, { "name": "p", "data": [ { "name": "text", "data": "CdSe/CdS量子点颗粒的尺寸和形态特征可通过透射电子显微镜进行表征，采用FEI TECNAI-G2F20和JEOL JEM-2100显微镜在200 kV(Cs 0.5 mm，点分辨率0.19 nm)下进行，用Gatan CCD相机记录图像。纳米颗粒从稀溶液中沉积到由200目铜网格支撑的厚度为3~4 nm的无定形碳膜上。将甲苯溶液中1~2滴纳米颗粒沉积在网格上，然后蒸发。光致发光发射谱和紫外-可见光吸收谱分别由F-4600(Hitachi)和UV-3600(Shimadzu)测试。X射线衍射图谱通过DY1602/Empyrean收集。漫反射光谱通过Cary 7000收集。荧光寿命曲线通过Quantaurus-Tau系统测试。荧光量子产率通过Quantaurus-QY系统进行测试。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3" } ], "title": [ { "name": "text", "data": "结果与讨论" } ], "level": "1", "id": "s3" } }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.1" } ], "title": [ { "name": "text", "data": "吸收与发射光谱表征" } ], "level": "2", "id": "s3a" } }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图1(a)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(a)" } ] } }, { "name": "text", "data": "显示了分散在甲苯溶液中CdSe/CdS量子点的光致发光发射谱和紫外-可见光吸收谱。由图可见，吸收光谱在505 nm附近有特征吸收峰，光致发光光谱峰唯一且对称，中心峰波长为517 nm，半峰宽为22.7 nm，光致发光量子产率为72.8%。从透射电子显微镜图像(" }, { "name": "xref", "data": { "text": "图1(a)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(a)" } ] } }, { "name": "text", "data": "中的插图)可以看出，CdSe/CdS量子点在甲苯溶液中的分散性较好。此外，我们通过对其中的50个纳米粒子进行粒径统计，得到" }, { "name": "xref", "data": { "text": "图1(b)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(b)" } ] } }, { "name": "text", "data": "粒径分布直方图。通过TEM图像和粒径分布统计图表明，CdSe/CdS核壳量子点的粒径尺寸约为6 nm。而且粒径分布符合预期的正态分布，尺寸分布均匀性较好。" } ] }, { "name": "fig", "data": { "id": "F1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图1" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS量子点的光致发光发射谱和紫外-可见光吸收谱；(b)CdSe/CdS量子点粒径分布直方图；(c)CdSe/CdS@PDMS-PUa复合材料的光致发光发射谱和紫外-可见光吸收谱；(d)CdSe/CdS@PDMS-PUa复合材料的光致发光均匀性表征。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 1" } ], "title": [ { "name": "text", "data": "(a)UV-Vis absorption and photoluminescence(PL) spectra of the CdSe/CdS quantum dots. (b)Statistical map of the particle size distribution. (c)UV-Vis absorption and PL spectra of the CdSe/CdS@PDMS-PUa composite. (d)Photoluminescence uniformity of CdSe/CdS@PDMS-PUa composites." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019880&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019882&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019881&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "PDMS-PUa共聚物中硅氧烷主链有着良好的疏水性能，这个特性将确保CdSe/CdS量子点的稳定性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "29", "type": "bibr", "rid": "R29", "data": [ { "name": "text", "data": "29" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。CdSe/CdS@PDMS-PUa复合材料是通过将CdSe/CdS量子点嵌入到PDMS-PUa聚合物中来制备的，CdSe/CdS量子点掺杂在PDMS-PUa中的质量浓度为0.8%。CdSe/CdS@PDMS-PUa复合材料的光致发光发射谱和紫外-可见光吸收谱如" }, { "name": "xref", "data": { "text": "图1(c)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(c)" } ] } }, { "name": "text", "data": "所示。吸收光谱也在505 nm附近有特征吸收峰。光致发光光谱的中心波长位于522 nm，半峰宽为22.4 nm，光致发光量子产率为41.9%。当将量子点溶液制备成量子点聚合物时，会出现福斯特共振能量转移现象，这将造成量子产率的显著降低" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "30", "type": "bibr", "rid": "R30", "data": [ { "name": "text", "data": "30" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。发射波长的红移主要来自甲苯溶剂蒸发，在一定程度上引起纳米粒子的聚集" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "31", "type": "bibr", "rid": "R31", "data": [ { "name": "text", "data": "31" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。从" }, { "name": "xref", "data": { "text": "图1(c)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(c)" } ] } }, { "name": "text", "data": "中的插图可以看到，CdSe/CdS@PDMS-PUa复合材料在365 nm紫外激发下可以观察到明亮的绿光。" }, { "name": "xref", "data": { "text": "图1(d)", "type": "fig", "rid": "F1", "data": [ { "name": "text", "data": "图1(d)" } ] } }, { "name": "text", "data": "为复合材料三个不同位置的光致发光光谱，三个位置的光致发光强度基本保持一致，说明了CdSe/CdS量子点在复合材料中的均匀分布。" } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "3.2" } ], "title": [ { "name": "text", "data": "荧光可逆分析" } ], "level": "2", "id": "s3b" } }, { "name": "p", "data": [ { "name": "text", "data": "众所周知，CdSe/CdS量子点本身可以通过各种机制降解，如水分、光降解、热降解，大大限制了其在光电器件方面的应用" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "32", "type": "bibr", "rid": "R32", "data": [ { "name": "text", "data": "32" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。我们将分散在甲苯溶液中的CdSe/CdS量子点旋涂于玻璃基板上，随后将CdSe/CdS量子点薄膜放置于水中，观测光致发光光谱的变化趋势。从" }, { "name": "xref", "data": { "text": "图2", "type": "fig", "rid": "F2", "data": [ { "name": "text", "data": "图2" } ] } }, { "name": "text", "data": "的变化趋势中发现，光致发光强度随着时间的推移逐渐降低，在24 h后降低到初始值的34%。其对水表现出较差的稳定性。" } ] }, { "name": "fig", "data": { "id": "F2", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图2" } ], "title": [ { "name": "text", "data": "CdSe/CdS量子点薄膜在水中的光致发光强度变化趋势" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 2" } ], "title": [ { "name": "text", "data": "Changing trend of PL intensity of CdSe/CdS quantum-dot film in water" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019884&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019900&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019899&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "与CdSe/CdS量子点薄膜相比，有聚合物包裹的CdSe/CdS量子点表现出一种完全不同的荧光现象。如" }, { "name": "xref", "data": { "text": "图3(a)、(b)", "type": "fig", "rid": "F3", "data": [ { "name": "text", "data": "图3(a)、(b)" } ] } }, { "name": "text", "data": "所示，制备的CdSe/CdS@PDMS-PUa复合材料在水中浸泡时，光致发光强度增强，同时伴随着荧光产率增大；然而从水中取出干燥后，光致发光强度减弱，同时也伴随着荧光产率减小。而且当我们循环地将复合材料进行水浸泡和取出干燥时，其荧光强度和量子产率表现出循环可逆的下降和上升规律。" } ] }, { "name": "fig", "data": { "id": "F3", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图3" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料多次循环水浸和干燥下光致发光强度的变化趋势；(b)CdSe/CdS@PDMS-PUa复合材料多次循环水浸和干燥下的量子产率变化趋势。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 3" } ], "title": [ { "name": "text", "data": "(a)Changing trend of PL intensity of CdSe/CdS@PDMS-PUa composite inmulti-cycled water immersion and air drying. (b)Changing trend of PLQY of CdSe/CdS@PDMS-PUa composite in in multi-cycled water immersion and air drying." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019902&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019891&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019890&type=" } ] } }, { "name": "p", "data": [ { "name": "xref", "data": { "text": "图4", "type": "fig", "rid": "F4", "data": [ { "name": "text", "data": "图4" } ] } }, { "name": "text", "data": "展示了CdSe/CdS@PDMS-PUa复合材料在水处理前后的扫描电子显微镜(SEM)图像，CdSe/CdS@PDMS-PUa复合材料的初始表面比较光滑，呈均匀分布的细沙状。水处理后，表面出现波纹和褶皱，这是由于水的进入导致了复合材料膨胀。通过复合材料前后形貌的改变可以验证水的进入。" } ] }, { "name": "fig", "data": { "id": "F4", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图4" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料水处理前的扫描电子显微镜图像；(b)CdSe/CdS@PDMS-PUa复合材料水处理后的扫描电子显微镜图像。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 4" } ], "title": [ { "name": "text", "data": "(a)The SEM images of CdSe/CdS@PDMS-PUa composite before water treatment. (b)The SEM images of CdSe/CdS@PDMS-PUa composite after water treatment." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019924&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019926&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019911&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步验证复合材料中存在水分子，" }, { "name": "xref", "data": { "text": "图5", "type": "fig", "rid": "F5", "data": [ { "name": "text", "data": "图5" } ] } }, { "name": "text", "data": "展示了CdSe/CdS@PDMS-PUa复合材料在水处理前后的傅里叶红外光谱，我们发现获得的傅里叶红外光谱曲线非常相似。然而，水处理后的傅里叶红外光谱以3 400 cm" }, { "name": "sup", "data": [ { "name": "text", "data": "-1" } ] }, { "name": "text", "data": "为中心有个宽峰，对应于官能团—OH，这无疑证实了复合材料中水分子的存在。" } ] }, { "name": "fig", "data": { "id": "F5", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图5" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料水处理前的傅里叶红外光谱；(b)CdSe/CdS@PDMS-PUa复合材料水处理后的傅里叶红外光谱。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 5" } ], "title": [ { "name": "text", "data": "(a)Fourier transform infrared(FTIR) spectrum of the CdSe/CdS@PDMS-PUa composite before water treatment. (b)Fourier transform infrared(FTIR) spectrum of the CdSe/CdS@PDMS-PUa composite after water treatment." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019914&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019931&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019930&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了探索荧光上升与水渗透的因果关系，我们首先测定了CdSe/CdS@PDMS-PUa复合材料放置于水前后的X射线衍射图谱，判断是否会出现晶格结构的变化。" }, { "name": "xref", "data": { "text": "图6", "type": "fig", "rid": "F6", "data": [ { "name": "text", "data": "图6" } ] } }, { "name": "text", "data": "分别将初始阶段的CdSe/CdS@PDMS-PUa复合材料、置于水后的CdSe/CdS@PDMS-PUa复合材料X射线衍射图谱与CdSe(PDF#08-0459)和CdS(PDF#41-1049)的标准理论峰位置进行了比较。一方面，通过横向比较，复合材料中的量子点的衍射峰与两个标准卡片的衍射峰都较为契合，说明不管是水处理前还是水处理后复合材料的量子点还是保持着良好的晶格结构" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "13", "type": "bibr", "rid": "R13", "data": [ { "name": "text", "data": "13" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "；另一方面，从轴向比较，水处理前后复合材料的X射线衍射图谱衍射峰位置和形状几乎不发生变化。由此可以进一步说明水处理并没有改变复合材料内部量子点的晶格结构。" } ] }, { "name": "fig", "data": { "id": "F6", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图6" } ], "title": [ { "name": "text", "data": "水处理前后的CdSe/CdS@PDMS-PUa复合材料X射线衍射图谱" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 6" } ], "title": [ { "name": "text", "data": "X-ray diffraction patterns of CdSe/CdS@PDMS-PUa composite before and after water treatment" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019917&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019935&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019919&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "此外，" }, { "name": "xref", "data": { "text": "图7(a)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(a)" } ] } }, { "name": "text", "data": "为一次循环过程中的三个不同阶段的光致发光光谱，经过比较发现，三个不同阶段的半峰宽和中心波长均没有发生太大的变化。其中，初始阶段的中心波长为522.2 nm，半峰宽为22.4 nm；浸入水中的中心波长为522.3 nm，半峰宽为22.5 nm；干燥后的中心波长为522.3 nm，半峰宽为22.4 nm。" }, { "name": "xref", "data": { "text": "图7(b)", "type": "fig", "rid": "F7", "data": [ { "name": "text", "data": "图7(b)" } ] } }, { "name": "text", "data": "显示，在多次循环过程中，CdSe/CdS@PDMS-PUa复合材料的中心波长位置和半峰宽的大小都保持相对稳定。这一观察结果从一定程度上也可以反映出CdSe/CdS量子点的晶格结构保持相对稳定" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "33", "type": "bibr", "rid": "R33", "data": [ { "name": "text", "data": "33" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F7", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图7" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料在一次循环过程中三个不同阶段(初始状态、水浸、干燥)的光致发光光谱；(b)CdSe/CdS@PDMS-PUa复合材料多次循环水浸和干燥下中心波长和半峰宽的变化趋势。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 7" } ], "title": [ { "name": "text", "data": "(a)PL spectra of the CdSe/CdS@PDMS-PUa composite at three different stages(initial state, water immersion, drying) during one cycle. (b)Changing trend of peak wavelength, FWHM of CdSe/CdS@PDMS-PUa composite in multi-cycled water immersion and air drying." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019940&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019944&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019943&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "由于这些CdSe/CdS量子点的尺寸很小，拥有相对大的表面积，因此在粒子表面存在着许多表面缺陷，晶体表面的缺陷态是限制其发光效率的重要因素" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "34", "type": "bibr", "rid": "R34", "data": [ { "name": "text", "data": "34" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。有文献报道水分子中一定程度的H" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "O" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "和OH" }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] }, { "name": "text", "data": "有利于钝化量子点的表面缺陷态" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "35", "type": "bibr", "rid": "R35", "data": [ { "name": "text", "data": "35" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "，我们推断导致荧光上升的原因可能是量子点表面缺陷态的钝化。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了验证这一猜想，我们测定了CdSe/CdS@PDMS-PUa复合材料在三个不同状态下的荧光衰减曲线，如" }, { "name": "xref", "data": { "text": "图8", "type": "fig", "rid": "F8", "data": [ { "name": "text", "data": "图8" } ] } }, { "name": "text", "data": "所示。荧光寿命的长短可反映表面缺陷态的程度。当粒子表面存在大量缺陷态时，这些缺陷态可作为无辐射跃迁的通道，使非辐射跃迁的速率增大，从而使荧光寿命减小。所以越长的荧光寿命对应越少的表面缺陷" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "36", "type": "bibr", "rid": "R36", "data": [ { "name": "text", "data": "36" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "38", "type": "bibr", "rid": "R38", "data": [ { "name": "text", "data": "38" } ] } } ], "rid": [ "R36", "R37", "R38" ], "text": "36-38", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。荧光衰减曲线拟合结果如" }, { "name": "xref", "data": { "text": "表1", "type": "table", "rid": "T1", "data": [ { "name": "text", "data": "表1" } ] } }, { "name": "text", "data": "所示。" } ] }, { "name": "fig", "data": { "id": "F8", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图8" } ], "title": [ { "name": "text", "data": "CdSe/CdS@PDMS-PUa复合材料在三个不同阶段(初始状态、水浸、干燥)的荧光衰减曲线" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 8" } ], "title": [ { "name": "text", "data": "Fluorescent decay curves of CdSe/CdS@PDMS-PUa composite at different stages(initial state, water immersion, drying)" } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019958&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019964&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019948&type=" } ] } }, { "name": "table", "data": { "id": "T1", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "表1" } ], "title": [ { "name": "text", "data": "荧光衰减曲线拟合结果" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Tab. 1" } ], "title": [ { "name": "text", "data": "Fitting results of fluorescence decay curves" } ] } ], "note": [], "table": [ { "head": [ [ { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "CdSe/CdS@PDMS-PUa" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "1" } ] }, { "name": "text", "data": "/ns" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "/ns" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-top:1px solid #000;border-bottom:1px solid #000;", "data": [ { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "avg" } ] }, { "name": "text", "data": "/ns" } ] } ] ], "body": [ [ { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "Initial state" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "127.23" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "42.35" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "10 224.11" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "0.21" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "31.8" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "Immersed in water" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "9 991.36" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "25.13" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "391.62" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "196.58" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "data": [ { "name": "text", "data": "59.6" } ] } ], [ { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "Drying in air" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "125.02" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "45.99" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "10 210.30" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "0.18" } ] }, { "colspan": "1", "rowspan": "1", "align": "center", "style": "border-bottom:1px solid #000;", "data": [ { "name": "text", "data": "32.1" } ] } ] ], "foot": [] } ], "graphics": { "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019969&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019967&type=" } } }, { "name": "p", "data": [ { "name": "text", "data": "平均荧光寿命" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "sub", "data": [ { "name": "text", "data": "avg" } ] }, { "name": "text", "data": "可采用如下公式进行计算：" }, { "name": "dispformula", "data": { "label": [ { "name": "text", "data": "(1)" } ], "data": [ { "name": "math", "data": { "graphicsData": { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019984&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019985&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019976&type=" } } } ], "id": "DF1" } }, { "name": "text", "data": "其中，" }, { "name": "italic", "data": [ { "name": "text", "data": "A" } ] }, { "name": "text", "data": "为拟合系数，" }, { "name": "italic", "data": [ { "name": "text", "data": "τ" } ] }, { "name": "text", "data": "为衰减时间。通过计算，初始状态下的平均荧光寿命为31.8 ns，放入水中后的平均荧光寿命为59.6 ns，干燥后的平均荧光寿命又恢复为32.1 ns。由此初步分析得出，在这个过程中，使得复合材料的光致发光强度出现上升的原因是CdSe/CdS量子点表面缺陷态的钝化，使得量子点的晶胞更趋于理想化，光学性能更好。然而，当CdSe/CdS@PDMS-PUa复合材料从水中取出干燥时，CdSe/CdS量子点表面缺陷态又重新暴露，所以CdSe/CdS@PDMS-PUa复合材料的光学性能又恢复到原来的状态。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "为了进一步验证这个可逆的机理与CdSe/CdS量子点表面缺陷的钝化和重暴露有关，我们还测定了CdSe/CdS@PDMS-PUa复合材料在三个不同阶段下的漫反射光谱。如" }, { "name": "xref", "data": { "text": "图9(a)", "type": "fig", "rid": "F9", "data": [ { "name": "text", "data": "图9(a)" } ] } }, { "name": "text", "data": "所示，三个阶段下的漫反射曲线非常相似，具有尖锐的吸收边缘，这归因于从价带顶部到导带底部的电子跃迁。初始状态下的CdSe/CdS@PDMS-PUa复合材料在571 nm处具有吸收边。当浸泡于水中后，复合材料的吸收边红移至539 nm。干燥后，吸收边移回572 nm。利用Kubelka-Mumk方程对Tauc图计算三个阶段的相应光学带隙，如" }, { "name": "xref", "data": { "text": "图9(b)", "type": "fig", "rid": "F9", "data": [ { "name": "text", "data": "图9(b)" } ] } }, { "name": "text", "data": "所示，三个阶段分别为2.19,2.30,2.18 eV。当粒子表面存在着许多晶格损伤(缺陷或陷阱、断键、悬键等)或吸附分子时，电子跃迁时的能量势垒较低，进而会表现出较小的光学带隙。因为光学带隙是光与物质相互作用时，物质中电子跃迁时的能量势垒" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "blockXref", "data": { "data": [ { "name": "xref", "data": { "text": "39", "type": "bibr", "rid": "R39", "data": [ { "name": "text", "data": "39" } ] } }, { "name": "text", "data": "-" }, { "name": "xref", "data": { "text": "41", "type": "bibr", "rid": "R41", "data": [ { "name": "text", "data": "41" } ] } } ], "rid": [ "R39", "R40", "R41" ], "text": "39-41", "type": "bibr" } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。当晶格损伤或者吸附分子消失后，光学带隙也会出现相应的增加。从光学带隙的变化趋势也可以很好地解释水处理消除了这些表面缺陷，而当水消失后，缺陷态又重新暴露" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "35", "type": "bibr", "rid": "R35", "data": [ { "name": "text", "data": "35" } ] } }, { "name": "text", "data": "," }, { "name": "xref", "data": { "text": "42", "type": "bibr", "rid": "R42", "data": [ { "name": "text", "data": "42" } ] } }, { "name": "text", "data": "］" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F9", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图9" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料在三个不同阶段(初始状态、水浸、干燥)的漫反射光谱；(b)使用Kubelka-Mumk函数绘制漫反射光谱的Tauc图。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 9" } ], "title": [ { "name": "text", "data": "(a)Diffuse reflectance spectra(DRS) of CdSe/CdS@PDMS-PUa composite at different stages(initial state, water immersion, drying). (b)Tauc plot using the Kubelka-Mumk function for DRS." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019988&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019982&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019989&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "为了探究CdSe/CdS@PDMS-PUa复合材料在长时间水浸和干燥的环境下，CdSe/CdS量子点表面缺陷态的钝化和暴露随时间变化的情况，我们测试了复合材料在长时间水浸和干燥下的光致发光强度和荧光光谱变化趋势。如" }, { "name": "xref", "data": { "text": "图10", "type": "fig", "rid": "F10", "data": [ { "name": "text", "data": "图10" } ] } }, { "name": "text", "data": "所示，AE段为CdSe/CdS@PDMS-PUa复合材料长时间放入水中荧光强度的变化曲线。我们发现，在CdSe/CdS@PDMS-PUa复合材料放入水中的前36 h(AC)，荧光强度一直处于上升阶段，但是上升的速率逐渐降低。我们分析这个现象的原因可能在于：靠近复合材料表层的量子点更快而且更容易接触到水分子，所以在前12 h内，荧光上升得很快；然而由于较少的水分子能够进入到复合材料深处，而且进入的速率相对较慢，所以位于深处的量子点被钝化的速率变得平缓。在36 h后，荧光出现了轻微下降(CD)，原因可能是由于小部分量子点表面会被吸附的水分子氧化而引入新的缺陷从而降低发光" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "43", "type": "bibr", "rid": "R43", "data": [ { "name": "text", "data": "43" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。然而随着时间的推移，复合材料内部的量子点趋于稳定的状态，所以荧光强度也趋于稳定(DE)。当重新把复合材料从水中取出，荧光强度重新恢复到初始值附近(EG)。我们发现，长时间的水浸并不会导致明显的荧光下降，总体来说，水对复合材料的作用还是体现为缺陷态的钝化，并没有破坏量子点的表面和核心，使量子点的光学性能出现持续降低。这得益于量子点外面包覆的高分子聚合物PDMS-PUa有着稳定的网络结构和较好的疏水性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "44", "type": "bibr", "rid": "R44", "data": [ { "name": "text", "data": "44" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "fig", "data": { "id": "F10", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图10" } ], "title": [ { "name": "text", "data": "(a)CdSe/CdS@PDMS-PUa复合材料长时间水浸和空气干燥的光致发光强度变化趋势；(b)CdSe/CdS@PDMS-PUa复合材料长时间水浸和空气干燥的光致发光光谱变化趋势。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 10" } ], "title": [ { "name": "text", "data": "(a)Changing trend of PL intensity of theCdSe/CdS@PDMS-PUa composite for long-time water immersion and air drying. (b)Changing trend of PL spectrum of the CdSe/CdS@PDMS-PUa composite for long-time water immersion and air drying." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019998&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28020002&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28019994&type=" } ] } }, { "name": "p", "data": [ { "name": "text", "data": "因此，对于裸露的量子点薄膜，与水的剧烈接触会迅速损坏量子点的表面和核心，并使量子点的光学性能出现持续降低。然而，当对量子点进行聚合物包覆保护后，量子点与水接触程度大大降低，本文中的PDMS-PUa起到阻挡作用，避免了水与量子点的剧烈接触。但是一定的水分子还是会通过聚合物网络基质的空隙接触到量子点，从扫描电子显微镜(SEM)和傅里叶红外光谱表征可以证实水分子的进入。但是进入的水分子不足以破坏量子点的结构，反而有利于量子点表面缺陷的钝化。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "通常，由于有机配体的空间位阻和材料化合物(如CdSe和CdS)的弱键合，量子点在合成阶段会导致形成较多的表面缺陷。此外，量子点与质子溶剂相互作用，例如乙醇和甲苯等，在离心和再分散步骤中也会导致表面配体脱离，形成缺陷。再者，在我们制备CdSe/CdS@PDMS-PUa复合材料的过程中，CdSe/CdS量子点与聚合物的混合搅拌也会导致表面配体脱离，形成缺陷。表面上的这些缺陷充当电荷载体的陷阱状态，导致非辐射激子重组并降低量子产率和光学特性。然而，当量子点与水分子接触时，这些陷阱态会通过H" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "O" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "和OH" }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] }, { "name": "text", "data": "钝化，使电子重新聚集在导带中，从而增强量子点的光学特性" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "27", "type": "bibr", "rid": "R27", "data": [ { "name": "text", "data": "27" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。当H" }, { "name": "sub", "data": [ { "name": "text", "data": "3" } ] }, { "name": "text", "data": "O" }, { "name": "sup", "data": [ { "name": "text", "data": "+" } ] }, { "name": "text", "data": "和OH" }, { "name": "sup", "data": [ { "name": "text", "data": "-" } ] }, { "name": "text", "data": "消失后，表面缺陷态又重新暴露，量子点的荧光产率和光学性能又恢复到初始值。" } ] } ] } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "4" } ], "title": [ { "name": "text", "data": "液体传感应用" } ], "level": "1", "id": "s4" } }, { "name": "p", "data": [ { "name": "text", "data": "量子点复合材料的荧光可逆性可拓宽其在光电领域的应用前景。而且所制备的聚合物复合材料不仅保留了PDMS的弹性、拉伸性等特性，其内部存在的大量动态氢键使其具有优异的自修复能力，这为CdSe/CdS@PDMS-PUa复合材料的应用奠定了坚实的基础" }, { "name": "sup", "data": [ { "name": "text", "data": "[" }, { "name": "xref", "data": { "text": "45", "type": "bibr", "rid": "R45", "data": [ { "name": "text", "data": "45" } ] } }, { "name": "text", "data": "]" } ] }, { "name": "text", "data": "。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "正如前文所讨论的，当CdSe/CdS@PDMS-PUa量子点复合材料遇水时，CdSe/CdS量子点的表面缺陷态被钝化，表现出荧光上升的趋势；然而有趣的是，当复合材料上的水消失后，CdSe/CdS量子点的表面缺陷态又重新暴露，表现出荧光下降的趋势。这种可逆的荧光上升和下降为实现对液体的光学传感创造了可能性。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "我们将CdSe/CdS@PDMS-PUa复合材料贴于烧杯的侧壁上，CdSe/CdS@PDMS-PUa复合材料的高度为15 mm，示意图如" }, { "name": "xref", "data": { "text": "图11(a)", "type": "fig", "rid": "F11", "data": [ { "name": "text", "data": "图11(a)" } ] } }, { "name": "text", "data": "所示。当复合材料接触到水的地方，荧光强度上升；而没有接触到水的地方，荧光强度不变(如" }, { "name": "xref", "data": { "text": "图11(a)", "type": "fig", "rid": "F11", "data": [ { "name": "text", "data": "图11(a)" } ] } }, { "name": "text", "data": "中插图所示)。利用CdSe/CdS@PDMS-PUa复合材料的亮暗分布可以实现对液面高度的预判。然而需要指出的是，我们还发现可以根据复合材料的荧光强度值来判断液面的具体高度。" }, { "name": "xref", "data": { "text": "图11(b)", "type": "fig", "rid": "F11", "data": [ { "name": "text", "data": "图11(b)" } ] } }, { "name": "text", "data": "显示了当液面处于不同高度时，在一定时间内复合材料荧光上升的程度。当液面高度越高，复合材料整体的光致发光强度上升的程度越大。这是由于更多的CdSe/CdS量子点被钝化，所以上升的程度越大。我们对不同液面高度的荧光强度进行拟合，如" }, { "name": "xref", "data": { "text": "图11(c)", "type": "fig", "rid": "F11", "data": [ { "name": "text", "data": "图11(c)" } ] } }, { "name": "text", "data": "所示，复合材料的荧光强度与液面高度成线性关系，且拟合优值" }, { "name": "italic", "data": [ { "name": "text", "data": "R" } ] }, { "name": "sup", "data": [ { "name": "text", "data": "2" } ] }, { "name": "text", "data": "达到了0.995。以上结果说明该复合材料的荧光强度可以用于来推断液面的具体高度。" } ] }, { "name": "fig", "data": { "id": "F11", "caption": [ { "lang": "zh", "label": [ { "name": "text", "data": "图11" } ], "title": [ { "name": "text", "data": "(a)基于CdSe/CdS@PDMS-PUa复合材料的液面高度传感器示意图；(b)不同液面高度下CdSe/CdS@PDMS-PUa复合材料的荧光变化规律；(c)液面高度与CdSe/CdS@PDMS-PUa复合材料荧光强度的线性拟合。" } ] }, { "lang": "en", "label": [ { "name": "text", "data": "Fig. 11" } ], "title": [ { "name": "text", "data": "(a)Schematic diagram of liquid level sensor based on CdSe/CdS@PDMS-PUa composite. (b)PL intensity variation of CdSe/CdS@PDMS-PUa composites at different liquid level. (c)Linear fitting of liquid level and PL intensity of CdSe/CdS@PDMS-PUa composite." } ] } ], "subcaption": [], "note": [], "graphics": [ { "print": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28020013&type=", "small": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28020017&type=", "big": "http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=28020005&type=" } ] } } ] }, { "name": "sec", "data": [ { "name": "sectitle", "data": { "label": [ { "name": "text", "data": "5" } ], "title": [ { "name": "text", "data": "结论" } ], "level": "1", "id": "s5" } }, { "name": "p", "data": [ { "name": "text", "data": "本文通过将核壳CdSe/CdS量子点封装到PDMS-PUa聚合物基质中制备了CdSe/CdS@PDMS-PUa复合材料，发现了其光致发光和量子产率的水致增强现象。然而，当该复合材料从水中取出后，其光致发光和量子产率都可以恢复到初始值，表明CdSe/CdS@PDMS-PUa量子点复合材料具有对水的荧光可逆现象。基于此，初探了一种具有荧光响应的液面高度光学传感器，通过荧光亮度的变化可以判断容器内液体的高度值。本文研究结果有助于对量子点的水致发光特性的深入理解，对其在光电器件中的应用奠定了重要基础。" } ] }, { "name": "p", "data": [ { "name": "text", "data": "本文专家审稿意见及作者回复内容的下载地址：http://cjl.lightpublishing.cn/thesisDetails#10.37188/CJL.20210401." } ] } ] } ], "footnote": [], "reflist": { "title": [ { "name": "text", "data": "参考文献：" } ], "data": [ { "id": "R1", "label": "[1]", "citation": [ { "lang": "en", "text": [ { "name": "text", "data": "JANG E" }, { "name": "text", "data": ", " }, { "name": "text", "data": "JUN S" }, { "name": "text", "data": ", " }, { "name": "text", "data": "JANG H" }, { "name": "text", "data": ", " }, { "name": "text", "data": "et al" }, { "name": "text", "data": ". 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