Two-Sidedness, Flexible, Durable, Highly Transparent and Haze Plastic-Paper For Green Optoelectronics

doi:10.21203/rs.3.rs-1034327/v1

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Two-Sidedness, Flexible, Durable, Highly Transparent and Haze Plastic-Paper For Green Optoelectronics

https://doi.org/10.21203/rs.3.rs-1034327/v1

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We combine biodegradable plastic (polyvinyl alcohol/glycerol polymer), and cellulose-based tissue paper in a very short time (5 s) by a facile way to form a new matrix, named plastic-paper, which has high optical transmittance (~89%) and high optical haze (~90%) in broadband. Results showed that the plastic-paper is durable in different solvents, with high folding strength (over 3500 folding times) and good mechanical strength (＞30 MPa tensile strength). Interestingly, the plastic-paper presents a two-sidedness of surface morphology. The rough side shows high light transmittance and the smooth side presents high optical haze. The smooth side of the plastic-paper is successfully applied to Organic Light-Emitting Diode (OLED). When the rough surface of plastic-paper is used in solar cells, the maximum output power increases by 2.6% compared with bare solar cells. The developed plastic-paper with high optical transmittance and high optical haze holds a great potential in flexible optoelectronic devices.

Polymer Science

Cellulose

Plastic-paper

Paper

Green

Flexible electronics have an excellent application prospect in medical, information and electronic fields(Z Fang et al. 2014; Reineke et al. 2009; Triambuloet alKimPark 2019; H L Zhu et al. 2013). For flexible electronic devices such as organic light-emitting diode (OLED) and solar cells, substrates play an important role(Han et al. 2012; KarimMonti 2021; Scholz et al. 2012; Wang et al. 2014; Zhou et al. 2012). Ideal substrates should have high transparency, high haze, good mechanical strength, flat and smooth surface, and can be manufactured in a cheap and convenient way(J Y Chen et al. 2015; Isogaiet alSaitoFukuzumi 2011; Nogiet alKomodaet alOtsukaSuganuma 2013; SulingOptoelectronics 2017). Nowadays, plastics are commonly used as flexible substrates for such electronic devices. However, the plastic substrate only transmits light, which limits its ability in light management(Butchosa et al. 2013; Fuet alAnsariet alZhouBerglund 2018; Layet alMendezet alDelgado-Aguilaret alBunVilaseca 2016). For example, only about 20% of the lights reach to OLED after multiple reflections and scattering using plastic substrates, even if the internal quantum efficiency is close to 100%. In addition, plastic will cause serious environmental pollution after discarding as wastes(Chehadi et al. 2021; Z Q Fang et al. 2014; Reineke et al. 2009; H Zhu et al. 2013; H L Zhu et al. 2016). Many researchers designed additional light management layers for OLED devices without light coupling capability on plastic and glass substrates. It has been found that the optical coupling ability of optoelectronic devices can be effectively improved by eliminating the interface scattering or having a transparent substrate with built-in high haze(Z Fang et al. 2014; Haet alFanget alHuMunday 2014; Wei et al. 2015; Zhu et al. 2016; H L Zhu et al. 2016; H L Zhu et al. 2013). However, all of these processes introduce additional manufacturing steps (film deposition and subwavelength structure) to increase the cost or produce some harmful wastes(Gieseet alBluschet alKhanMacLachlan 2015; Kellyet alLantet alKurrBurgess 2019).

Recently, sustainable cellulose materials show a great potential in electronic products(Chenget alZhanget alLaiHuang 2015; L B Hu et al. 2013; Jung et al. 2015; Mazaheriet alLeeet alvan der Zantet alFrisendaCastellanos-Gomez 2020; MoragJelinek 2016; Tanget alButchosaZhou 2015) due to their good flexibility, extensibility, and degradability. As the most abundant renewable polymers on the earth, cellulose and its products are ubiquitous in our life, but their wider application is usually limited by the electrical insulation, high opacity and low mechanical strength(S Chenet alSongXu 2018; FagiolariBella 2019; Hou et al. 2020; Iwamiyaet alKawaiet alNishio-Hamaneet alShibayamaHiroi 2020; Kansalet alHamdaniet alPinget alSirinakbumrungRabnawaz 2020). Through chemical modification, reconfiguration or integration with other nanomaterials, cellulose paper becomes the most promising plastic substitutes(S Chen et al. 2018; Fouratiet alMagninet alPutauxBoufi 2020; W Hu et al. 2018; Kansal et al. 2020; Mateos-Cardenaset alO'Halloranet alvan PeltJansen 2021; Yao et al. 2016; ZhangToudert 2018; M W Zhu et al. 2016). Tissue paper is made of cellulose with good optical haze and flexibility. However, the transparency and mechanical strength of tissue paper itself are obviously insufficient. Consequently, it is vital to modify the tissue paper by combining with other renewable substrates with high transparency and good mechanical strength.

Here, we choose a convenient and scalable method to composite single-layer cellulose-based tissue paper with polymer solution to form the plastic-paper. Plastic-paper is made of a single layer of tissue paper as a skeleton through the penetration of Polyvinyl alcohol (PVA) and glycerol by template transfer method. The degradable material formed by the infiltration of polymer and single-layer tissue paper has a sandwich structure, which combines the advantages of these two materials and makes them have unique optical properties. Due to the different roughness of two sides of the plastic-paper with unique properties of light transmittance and optical haze, the plastic-paper can be applied in OLED and solar cells. Furthermore, the plastic-paper shows good flexibility like tissue paper, but its mechanical strength is at least hundreds of times higher than tissue paper. The developed plastic-paper with excellent properties and facile preparation process make it have a bright future in a series of flexible electronic materials.

2.1 Materials

Polyvinyl alcohol (PVA, polymerization degree of 1,750 ± 50) was purchased from Sinopharm Chemical Reagent Co., Ltd., China. Glycerol was purchased from Tianjin Fuyu Fine Chemical Co., Ltd., China. The cellulose-based tissue paper (100% Native wood pulp) came from ZhongShun JieRou paper industry (paper basis weight is 16 g/m²).

2.2 Fabrication of plastic-paper

A simple solution permeation method was used to prepare plastic mixed paper membrane (plastic-paper). 10 g of PVA, 4.3 g of glycerol and 90 mL of deionized water were added into a flask with a thermometer and a mechanical stirrer. The mixtures were heated to 92 ℃ ± 2 ℃ for 3 h until completely dissolved. Subsequently, the prepared polymer solution was taken out and cooled to room temperature. Slowly put the single-layer tissue paper into the PVA solution, fully immerse the single-layer tissue paper in the solution for 5S, and slowly take it out. Transfer the impregnated single-layer tissue paper and polymer (50 wt%) to a smooth glass plate and flatten it with a glass rod. Finally, the glass plate was put into the oven directly at 60 ℃ and dried for 5 minutes to obtain the plastic-paper with two-sidedness.

2.3 Evaluation of plastic-paper

The thickness of plastic-paper was determined by a thickness tester (L&W, Sweden). Scanning electron microscope (SEM) measurements were carried out on an EVO 18 SEM (Carl Zeiss, Germany) with a voltage of 10 kV. Ultra-depth three-dimensional microscope was observed on VHX-700F (Keith Co., Ltd, Japan). Atomic force microscope (AFM) measurements were performed on a digital instrument multimode in tapping mode (Rigaku, Japan). Optical transmittance and haze were measured on a LAMBDA 1050 UV/Vis/NIR spectrophotometer with an integrated sphere. Strain-stress curves were obtained by a 5565 universal material experiment machine (Instron, Boston, U.S.A.). The sample strip with the size of 15×100 mm is pulled with a constant force of 9.8 N and repeatedly folded to 180° until it breaks from the folding line. The air permeation rate was measured on an L&W 166 with a measurement size of 50 cm².

3.1 From cellulose-based tissue paper to plastic-paper

Tissue paper is composed of cellulose microfibers with small pores, resulting in a high surface roughness and a strong light scattering surface in the air, which also results in the high optical haze and low transparency. The PVA/glycerol polymer or film has strong hydrogen bonding, excellent mechanics, easy to degrade and solvent resistance. The uniform structure of the film also makes it very tough and transparent, thus has a low optical haze while high transmittance. Herein, through a simple template penetration method, we combine the three materials perfectly to achieve a novel degradable plastic-paper with a "sandwich" and sidedness structure, which provides excellent mechanical properties, high optical transmittance (~ 88%) and high optical haze (> 90%) (Fig. 1).

We use commercially available single-layer tissue paper as the paper substrate. The cellulose micro-pore structure inside the single layer of tissue paper allows the polymer to permeate rapidly to form the plastic-paper hybrid substrate. Here, a mixture of polyvinyl alcohol and glycerin was used as the infiltration polymer because its refractive index of 1.55 is very close to that of cellulose (1.54), thus ensuring minimal light scattering at the plastic-paper interface. Moreover, the PVA is modified by glycerol as plasticizer and the polymer has excellent transparency, biocompatibility and gas barrier property. Through the interaction with the hydroxyl groups on the PVA molecular chain, the hydrogen bonds between the hydroxyl groups of PVA is weakened, which can effectively improve the mechanical properties of PVA(Jianget alLuoet alHouZhao 2016). The polymer solution prepared by the mixture of PVA and glycerol has superior fluidity and low viscosity, which makes it easier to penetrate into the fiber pores of tissue paper. After curing, the polymer has good mechanical properties and solvent stability, which can protect the cellulose paper from being easily decomposed or broken by solvent in the process of material preparation. The glass plate is used as the plate template to ensure super flat surface transferring.

Images of the plastic-paper are shown in Fig. S1. The clear pattern at the bottom of the plastic-paper (plastic-paper attached to the background) indicates the high transparency of the plastic-paper, and the fuzzy pattern at the top (plastic-paper away from the background) indicates the high haze of the plastic-paper (Fig. S1c). In addition to this unique optical property, compared with the tissue paper, plastic-paper hybrid substrate also has excellent mechanical properties and two-sided properties, which is attributed to the hydrogen bonds formed by polymer and single-layer tissue paper. Plastic-paper also has excellent folding resistance and solvent stability, benefits from the "sandwich" structure formed by polymer and cellulose. The polymer in the outer layer provides a good encapsulation for the plastic-paper, and the polymer in the inner layer and cellulose fiber is crosslinked to form an interpenetrating network structure. The preparation of plastic-paper is based on the mature and industrialized technology, which makes this new type of plastic-paper being very promising and attractive for the high-performance, low-cost optoelectronic substrates.

3.2 Surface topography of plastic-paper

Templated penetration is to impregnate a single layer of tissue paper in PVA/glycerol polymer solution and transfer to the surface of smooth glass plate, and then dry it at a certain temperature. Through the template transfer, the lower surface of the plastic-paper contacting with the glass plate becomes flat and smooth, and the upper surface contacting with the air has a certain roughness (Fig. 2). Very smooth surface is observed on the polymer film (Fig. S2a). Contrarily, the micro-sized cellulose fibers of single-layer tissue paper are extruded into a flat and loose shape, and interwoven together to form a certain surface roughness of the paper (Fig. S2b). When the polymer solution is infiltrated, the lower surface of the plastic-paper becomes super flat and smooth due to contact with the glass plate and the porous surface is replaced by the dense and flat polymer (Fig. 2d). The upper surface of the plastic-paper has a certain roughness due to the contact with the air, which leads to the incomplete polymer substitution (Fig. 2a).

The cross section of single-layer tissue paper shows a loose fiber structure with micro-sized fibers and many pores (Fig. S2c). Plastic-paper shows a typical "sandwich" packaging structure (Fig. S2d). Both sides of the plastic-paper are encapsulated by the polymer solution to form a thin surface layer. The internal dense cellulose fiber and polymer are cross-linked to form an interpenetrating network structure. It can be seen that the polymer solution has well penetrated into the single-layer tissue paper, and the "sandwich" structure can greatly improve the mechanical properties of plastic-paper. In order to further characterize the surface roughness of plastic-paper, ultra-depth three-dimensional microscope is used and it can intuitively show that the lower surface of the plastic paper presents uniform blue color, indicating of the smoother Surface topography than the upper surface (Fig. 2b and 2e). AFM results show that lower surface roughness is approximately ~3.5 nm while upper surface roughness is ~45 nm, indicating of the two-sidedness property of the plastic-paper (Fig. 2c and 2f).

3.3 Optical Properties

The optical transmission characteristics of polymer film, single-layer tissue paper and plastic-paper are compared in Fig. 3a and 3b. Significantly different optical transmission characteristics are observed. Polymer film has the highest optical transmittance of ~92%. The smooth side (lower surface) of plastic-paper presents a total transmittance of ~89% from 300 nm to 800nm (broadband). The single-layer tissue paper substrate shows the lowest optical transmittance of less than 75%. The high transmittance of plastic-paper is in consequence of the increased material density and the smooth surface after polymer infiltration inside the porous tissue paper(Limet alRakuTokiwa 2004). The rough side (upper surface) of plastic-paper is equal to overall transmittance of ~85% from 300 nm to 800 nm. The optical duality is caused by the different roughness of two sides of plastic-paper. The higher surface roughness will increase the reflection area of light, which will affect the transmittance(Dai et al. 2014).

The polymer film shows the extremely optical haze below 10% (Fig. 3c). The tissue paper and plastic-paper show a high optical haze of ~90% from 300 nm to 800 nm (broadband), indicating that a great amount of lights are reflected and scattered as it passed through a single layer of tissue paper or plastic-paper. The light scattering effect or optical haze characteristic is display intuitively in the illustration (Fig. 3d). When the green laser passes through the plastic-paper, it shows a high intensity and high scattering light pattern on the white wall, indicating the excellent optical transmittance and high optical haze. The high haze of plastic-paper is due to the rough surface, loose porous fiber structure and polymer fiber interface with single layer tissue paper. The polymer coated plastic-paper can effectively reduce the backscattering of lights. Meanwhile, cellulose has mesoporous structure and polymer-fiber interface can cause forward scattering of transmitted light so that the plastic-paper has a very high optical haze (Dai et al. 2014), which is also the reason why the optical transmission haze characteristics of the two sides of the plastic-paper are different slightly. Due to the different roughness, the haze of the rough side (upper surface) of plastic-paper is larger than that of smooth side (lower surface) as shown in Fig. 3c and 3d.

The new plastic-paper developed in this study shows the advantages of both plastic and single-layer tissue paper. It shows high optical transmittance and high optical haze in the visible light range, which has the potential for improving the photoelectric conversion efficiency of solar cells and OLED. Usually, it is difficult for traditional substrate materials such as glass, silicon and plastic to have such excellent optical properties. A traditional light management method is to add a coating layer on the original transparent and smooth substrate to improve the optical haze (D Chenet alLiangPei 2016). However, this traditional method requires additional manufacturing steps and has limited enhancement capabilities. The developed plastic-paper can make up for the incompatibility of traditional optical materials. Even increasing the cellulose contents in plastic-paper from 30wt% to 50wt%, the plastic-paper still presents high optical transmittance and optical haze (Fig. S3).

3.4 Mechanical Properties.

In addition to its excellent optical properties, plastic-paper also possesses good mechanical properties and outstanding solvent stability, which is the key to direct device manufacturing. The stress-strain curves of single-layer tissue paper, polymer film and plastic-paper are given in Fig. 4a. The tensile strength (30 Mpa) and elongation at break (0.4 Mpa) of plastic-paper are the highest compared with that of tissue paper and polymer film. Plastic-paper can readily lift 1kg of reactor for more than 24h (Fig. S4b). Folding endurance is one of the basic mechanical properties of paper, which is used to express the ability of paper to resist reciprocating folding. Fig. 4b shows the excellent folding durability of plastic-paper. The results show that the longitudinal folding resistance of plastic-paper (3528 times) is far larger than that of tissue paper (15 times). Similarly, the transverse folding resistance (258 times) is also much higher than that of tissue paper (7 times). It is closely related to the "sandwich" structure of plastic-paper. Specifically, the polymer encapsulates the tissue paper on the outside. Polymer connects the cellulose in a single layer of tissue paper and fills the intervals between the cellulose fibers. The inner part of the plastic-paper is cross-linked with the cellulose fiber, and they interweave with each other to form an interpenetrating network structure. The fiber structure also enhances the composite effect of polymer matrix. It can significantly enhance the mechanical properties of plastic-paper, especially the tear resistance and folding resistance.

Compared to the original single-layer tissue paper, the plastic-paper significantly enhances the stability in solvents and water. As shown in Fig. 4c, after a three weeks water stability test, ordinary tissue paper is decomposed into cellulose fiber, while the plastic-paper keeps nice shape stability without any obvious changes. It is indicated that the polymer itself has good solvent resistance with relatively large contact angle (Fig. S4a) and binds the cellulose fibers together to prevent disintegration. Ordinary paper soaked in solvent and taken out to dry will expand and produce many wrinkles, which is a serious problem in the manufacture of microelectronic devices. We demonstrate the stability of plastic-paper in solvents required for the fabrication of optoelectronic devices, such as photoresist 1813 and acetone for 1 day (Fig. 4d). Plastic-paper has great shape retention and outstanding stability in these chemical reagents and organic solvent and therefore can be directly used for the purpose of flexible substrates requiring different solvents. The water and vapor permeation rate (WVPR) is critical for devices containing sensitive components such as conductive and semi-conductive polymers. Due to its good oil resistance and excellent gas barrier performance, PVA has unique advantages in food and drug packaging. By templated penetration, the plastic-paper substrate shows excellent WVPR of 0.5 g m⁻² day⁻¹.

3.5 Application in electronic devices

In order to prove the process compatibility and enhance the optical coupling of plastic-paper in optoelectronic devices, Electroluminescent (EL) devices are fabricated directly on plastic-paper. Ag NWs dispersion evenly coat in plastic rough surface (upper surface) to form a conductive network. The conductive film after coating is applied as the positive and negative pole of EL devices. EL light-emitting layer and insulating layer by means of silkscreen print on the conductive film. When the power supply is connected, the film shows blue fluorescence (Fig. 5a and 5b). Using the rough surface of plastic-paper as the substrate material of EL devices can make Ag NWs form a conductive network with strong adhesive force on the plastic-paper through a simple coating process. This application demonstrates the potential value of thin plastic-paper in the field of electronic devices.

Plastic-paper also has great application value in the field of solar cells due to its unique optical properties. The prepared plastic-paper is used as the anti-reflection layer on the solar cell, which contacts the smooth surface (lower surface) with the solar cell. The lower surface is flat and smooth, which can increase the effective contact area with the solar cell. The upper surface has a certain roughness, which can be used as the light trap of the solar cell, so that the light with a single small incidence angle can be scattered in all directions, thus increasing the light path in the solar cell and increasing the light absorption. This dual surface roughness can ultimately improve the photoelectric conversion efficiency of solar cells. The simple solar cells device is shown in Fig. 5c. The volt ampere characteristic curves of solar cells with or without plastic-paper are shown in Fig. 5d. After covering the solar cell with plastic-paper, the open circuit voltage increases from 7.01 V to 7.05 V, and the short circuit current increases from 130 mA to 134 mA. The filling factor increases from 64.23–64.66% with plastic-paper. It is indicated that plastic-paper can improve the light absorption efficiency of solar cells, not only improve the quantum efficiency, but also increase the short-circuit current and open circuit voltage of solar cells, leading to further improving the photoelectric conversion efficiency of solar cells.

We report a new and extremely simple method to convert ordinary cellulose-based tissue paper (single-layer) into plastic-paper. The developed plastic-paper presents high optical transmittance (~89%) and high optical haze (~90%) in broadband. The plastic-paper is successfully applied to the optoelectronic devices and solar cells. Compared with traditional substrates, it can improve the energy conversion efficiency of solar cells. The sustainable plastic-paper can be widely used as a durable, flexible and continuous bending substrate in green optoelectronics.

Acknowledgments

This work was supported by the Foundation (No. KF201917) of the Key Laboratory of Pulp and Paper Science and Technology of the Ministry of Education of China and by the National Natural Science Foundation of China (31800497).

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Reviews received at journal
14 Nov, 2021
Reviewers invited by journal
14 Nov, 2021
Editor invited by journal
13 Nov, 2021
Editor assigned by journal
01 Nov, 2021
First submitted to journal
30 Oct, 2021

You are reading this latest preprint version

Two-Sidedness, Flexible, Durable, Highly Transparent and Haze Plastic-Paper For Green Optoelectronics

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Abstract

Figures

1. Introduction

2. Material And Methods

2.1 Materials

2.2 Fabrication of plastic-paper

2.3 Evaluation of plastic-paper

3. Results And Discussion

3.1 From cellulose-based tissue paper to plastic-paper

3.2 Surface topography of plastic-paper

3.3 Optical Properties

3.4 Mechanical Properties.

3.5 Application in electronic devices

Conclusion

Declarations

Acknowledgments

References

Supplementary Files

Status:

Version 1