Preparation, properties and application of highly hazy and transparent cellulose films for solar cells
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摘要: 将可持续的纤维素材料与电子器件结合是当今学术界的研究热点。高雾度透明纤维素薄膜是一种具有特殊光学性能的纸张。它除了具有普通纸张的优点(可降解、成本低、柔性、质轻等)外，还呈现出高的透光率和优异的光散射性能，可作为绿色光学透明材料应用于太阳能电池，提升电池的光电转化效率。本文首先简要介绍了高雾度透明纤维素薄膜的发展历程；接着，详细总结了高雾度透明纤维素薄膜的制备方法及其性能(如光学、力学、热稳定性、耐水等)；然后论述了现阶段这类薄膜在太阳能电池中的应用进展；最后，总结了高雾度透明纤维素薄膜存在的科学技术问题，并对其今后的研究方向以及应用前景进行了展望。Abstract: Integrating sustainable cellulose materials into electronic devices is a hot research topic in academic communities. Highly transparent cellulose film with high transmission haze is a kind of paper with special optical properties. In addition to the advantages (degradability, low cost, flexibility, light weight, etc.) of ordinary paper, it also presents high transparency and strong light scattering behavior (high transmission haze), and has the potential to use in solar cells as a green optical transparent material to improve the power conversion efficiency. In this review, the development process of highly hazy and transparent cellulose film was first introduced. Then, the preparation and properties (such as optical properties, mechanical properties, thermal stability and water resistance) of highly transparent and hazy cellulose films were summarized in detail. After that, the progress in the use of transparent and hazy cellulose film in solar cells was discussed. Finally, scientific and technical problems of highly transparent and hazy cellulose films for solar cells were summarized, and their challenges and future research direction were provided as well.
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Key words:
- high transmission haze /
- high transparency /
- cellulose film /
- light scattering /
- solar cells
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图 1 光照射纤维素薄膜时的光线路径图
Figure 1. Diagram of light path when a light passes through the cellulose film
图 4 高雾度透明纤维素薄膜的制备方法：(a)真空抽滤法[9,35]；(b)铸涂法[39]；(c)涂布法[12]；(d)浸渍法[43]；(e)纤维表面选择性溶解法[31,45]；(f)“自上而下”法[32]
Figure 4. Preparation methods of highly hazy and transparent cellulose films: (a) Vacuum filtration[9,35]; (b) Casting[39]; (c) Coating[12]; (d) Impregnation[43]; (e) Surface selective dissolution[31,45]; (f) Top-down[32]
TEMPO—2,2,6,6-Tetramethylpiperidine-1-oxyl radical; TOCN—2,2,6,6-Tetramethylpiperidine-1-oxyl radical oxidized cellulose nanofibrils; TOWFs—TEMPO-oxidized wood fibers
图 5 一束光分别通过普通纸(a)、超清晰膜(b)、高雾度透明薄膜(c)所发生的反射、折射及散射现象[43]；(d)高雾度透明纤维素薄膜的照片[31]；高雾度透明纤维素薄膜(Hazy paper)与聚对苯二甲酸乙二酯(PET)、柔性玻璃(Flexible glass)的透光率(T) (e)及雾度(H)对比(f)[31]
Figure 5. Reflection, refraction, and scattering of a beam of light through common paper (a), ultra clear film(b), and highly hazy and transparent film[43]; (d) Photograph of highly hazy and transparent cellulose film[31]; Comparison of transmittance (T) (e) and haze (H) (f) of highly hazy and transparent cellulose film (Hazy paper), poly (ethylene terephthalate) (PET) and flexible glass[31]
图 6 (a)普通纸、羧甲基纤维素(CMC)膜以及高雾度透明复合膜的应力-应变曲线[43]；(b)各向异性高雾度透明薄膜和各向同性纳米纸的应力-应变曲线[33]；(c)普通纸、TEMPO-氧化纸、CMC膜以及高雾度透明复合膜的耐折度[43]；(d)高雾度透明复合膜和TEMPO-氧化纸的耐折性能比较[43]
Figure 6. (a) Stress-strain curves of common paper, carboxymethyl cellulose (CMC) film and highly hazy and transparent composite film[43]; (b) Stress-strain curves of anisotropic highly hazy and transparent film and isotropic nanopaper[33]; (c) Folding endurance of common paper, TEMPO-oxidized paper, CMC film, and highly hazy and transparent composite film[43]; (d) Folding measurement of highly hazy and transparent composite film and TEMPO-oxidized paper[43]
图 7 高雾度透明纤维薄膜的热稳定性：由木质纤维和CMC组成的高雾度透明薄膜、纯CMC薄膜、普通纸以及由TEMPO氧化木浆组成的高雾度透明薄膜的热重分析(a)和极限氧指数分析(LOI) (b)；(c)由木质纤维和CMC组成的高雾度透明薄膜(A)、纯CMC膜(B)、普通纸(C)由TEMPO氧化木浆组成的高雾度透明薄膜(D)的垂直燃烧测试[43]
Figure 7. Thermal stability of highly hazy and transparent cellulose film: Thermogravimetric (a) and Limiting oxygen index (LOI) (b) analysis of highly hazy and transparent composite film made by wood fibers and CMC, CMC film, common paper and TEMPO-oxidized paper; (c) Vertical flame testing of highly hazy and transparent composite film (A), CMC film (B), common paper (C) and TEMPO oxidized paper (D)[43]
图 8 高雾度透明纤维复合薄膜的耐水性能：(a)高雾度透明纤维素薄膜吸水率和厚度随时间的变化以及吸水率的拟合曲线；(b)高雾度透明纤维素薄膜长度和宽度随浸泡时间的变化；(c)普通纸和高雾度透明纤维素薄膜的初始水接触角(WCA)；(d)普通纸和高雾度透明纤维素薄膜在水中浸泡2小时后的照片；(e)普通纸、高雾度透明纤维素薄膜以及再生纤维素薄膜(RCF)的湿强度[34]
Figure 8. Water resistance of highly hazy and transparent cellulose composite film: (a) Water absorption and thickness change of composite film as a function of immersion time and corresponding fitting curves of time-dependent water absorption based on Box Lucas1 model; (b) Changes in length and width of composite film with increasing immersion time; (c) Original water contact angles (WCA) of paper and composite film; (d) Digital images of paper and composite film after immersing into water for two hours; (e) Wet strength of paper, composite film and RCF[34]
图 9 (a)贴有高雾度透明纤维素薄膜的有机太阳能电池的结构[9]；贴附高雾度透明纤维素薄膜前后有机太阳能电池(b)和砷化镓太阳能电池(c)的电流密度-电压曲线(W和W/O分别代表未贴膜有和贴薄[9]，插图为贴附高雾度透明纤维素薄膜的砷化镓太阳电池)；(d)贴附高雾度透明纤维素薄膜前后砷化镓太阳电池在全可见光波段、不同入射角条件下的光反射率；(e)太阳能电池上入射光分布的示意图[32]；(f)贴附高雾度透明纤维素薄膜前后砷化镓太阳能电池的电流密度-电压曲线[32]
Figure 9. (a) Structure of organic solar cells coated with highly hazy and transparent cellulose films[9]; Current densities-voltage curves of organic solar cells (b) and gallium arsenide (GaAS) solar cells (c) with (W) and without (W/O) highly hazy and transparent cellulose film[9]; (d) Optical reflectance of GaAs solar cells at different incidence angles and at all visible wavelengths before and after attaching highly hazy and transparent cellulose film[32]; (e) Schematic diagram of incident light distribution on a solar cell[32]; (f) Current densities-voltage curves of GaAs solar cells before and after attaching highly hazy and transparent cellulose film[32]
表 1 高雾度透明纤维素薄膜的制备与性能
Table 1. Preparation and properties of highly hazy and transparent cellulose films
Material Film
namePretreat-
mentPreparation
methodPreparation
timeT and H Mechanical
propertyThermo-
stabilityWater
resistanceRef. Northern wood pulp and CMC All-cellulose composite films — Impregnation >5 h T: 90%;
H: 82%Tensile stress:
140 MPa;
Toughness:
8.5 MJ·m−3;
Folding times:
3342Td: 254℃; LOI: 30% CA: 43° [43] Northern wood pulp and CMC Transparent and hazy paper — Impregnation + protonation >10 h T: 91%;
H: 84%Tensile stress:
108 MPa;
Folding times: 994— CA: 72°; Saturated water Absorptivity: 60%; Change in thickness: 25% [67] Bleached softwood kraft pulp Hazy TOCN films TEMPO oxidation + homogeni-
zationCasting + coating >24 h T: 85%;
H: 62%— — — [12] Bleached softwood kraft pulp Highly translucent and light-diffusive film TEMPO oxidation + homogeni-
zationCasting >12 h T: 90%;
H: 78%— — — [25] Bleached softwood kraft pulp Ag NW paper TEMPO oxidation + homogeni-
zationVacuum filtration — T: 91%;
H: 65%— — — [29] Bleached softwood pulp Highly transparent and hazy paper — Surface selective dissolution >8 h T: 90%;
H: 91%— — — [31] Bleached softwood kraft pulp Nanostruc-
tured paperTEMPO oxidation Vacuum filtration >10 h T: 96%;
H: 60%Tensile stress:
105 MPa— — [9] Basswood Anisotropic transparent paper — “Top-down” >8 h T: 90%;
H: 90%Tensile stress:
350 MPa; Toughness:
7.38 MJ·m−3— — [32] Basswood Anisotropic wood film — “Top-down” >8 h T: 90%;
H: 80%— — — [33] Northern wood pulp Highly transparent paper TEMPO oxidation Vacuum filtration >5 h T: 90%;
H: 84%Tensile stress:
89.2 MPa; Bursting strength: 85 MPa; Young's modulus: 7.73 GPa— — [39] Northern wood pulp Highly transparent paper TEMPO oxidation Casting 41-53 h T: 88%;
H: 72%Tensile stress:
85.3 MPa; Bursting strength: 124 MPa; Young's modulus: 12.89 GPa— — [39] Bleached softwood kraft pulp Highly hazy and transparent cellulose film Carboxy-
methylationVacuum filtration >2.5 h T: 89%;
H: 85%Tensile stress:
138 MPaTd: 179℃ — [40] Pine dissolving pulp Highly hazy transparent cellulose film TEMPO oxidation + ultrasoni-
cationCasting — T: 90%;
H: 76%Tensile stress:
22 MPaTd:
295-305℃;
CTE: 8.5-10.6 ppm/K— [78] Cellulose pulp Hazy transparent cellulose nanopaper Alkali treatment + homogeni-
zationVacuum filtration >10 h T: 90%;
H: 90%— — — [38] Bleached softwood pulp and CNF Bilayer hybrid paper TEMPO oxidation + homogeni-
zationVacuum filtration — T: 92%;
H: 70%— — — [23] Bleached softwood kraft pulp Nanostruc-
tured paperMicrofibrilla-tion Vacuum filtration >2.3 h T: 83%;
H: 89%Tensile stress:
18.5 MPa;
Young's modulus:
3.04 GPa— — [79] Bleached softwood kraft pulp Transparent and hazy all-cellulose composite films Impregnation >12 h T: 90%;
H: 95%Tensile stress: 37.03 MPa; Young's modulus: 1.90 GPa; Toughness:
2.78 MJ·m−3— CA: 76°; Saturated water Absorptivity: 59%; Change in thickness: 30% [34] Notes: CNF—Cellulose nanofibrils; Ag NW—Silver nanowire; Td—Thermal decomposition temperature; CTE—Coefficient of thermal expansion; CA—Contact angle. 
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