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The performance of solar cells using chlorophyll dye from Syzygium paniculatum

The performance of solar cells using chlorophyll dye from Syzygium paniculatum 3.5 SP-Red SP-Green 2.5 SP-Mix DSSC Process 1.5 0.5 300 400 500 600 700 800 Wavelength, nm FTO with TiO + PEG The relationship between wavelength and absorbance coating uses a 0.18 MPa spray gun Spectrum Ti Ti Counter electrode Ca Mg Si K Ca l Ti from carbon 0 0 123456789 keV EDX test result FTO-TiO / I V (V)V I (V) FF 2 sc SC max max –2 –2 PEG- Dye (mA.cm ) (mA.cm ) (%)(%) SP-Red 0.0039 0.258 0.003 0.15 44.723 1.102 DSSC (Electrode + Electrolyte + Counter SP-Green 0.0047 0.432 0.0039 0.39 74.911 3.724 electrode) SP-Mix 0.0048 0.323 0.0039 0.25 62.887 2.387 FF value and DSSC performance Keywords: chlorophyll; flavonoids; photoanode TiO ; solar cell; Syzygium paniculatum Further, the porphyrin dyes were evaluated as the sen- Introduction sitizers of DSSCs based on an I/I electrolyte, increasing 2 3 Dye-sensitized solar cell (DSSC) technology is a third- efficiency dramatically to 11.5% [12]. Making DSSC (XW28) generation dye-based solar cell technology with easy fabri- using porphyrin dye by inserting a chain into its appro- cation, low production costs and environmentally friendly priate position of the benzothiadiazolyl acceptor section [1–5] silicon-based solar cells. However, silicon-based solar resulted in a high efficiency of 10.14% [13]. Higashino re- cells have several disadvantages: pure silicon, high tech- viewed research using porphyrin dyes to increase effi- nology, dangerous chemicals and high prices. Therefore, ciency by ≤13% [14]. Development of a synthetic organic researchers are interested in developing DSSCs. The dyes dye Z2 linked to a double-bond porphyrin dye and added used today are synthetic dyes and natural dyes. Synthetic with chenodeoxycholic acid (CDCA), XW61 provided 12.4% dyes such as the ruthenium complex contain heavy metals efficiency [15]. that are less favourable in the environment [6]. Due to such Moreover, solar cells with TiO material are essen- difficult and expensive designation, researchers look for tial factors that determine the photovoltaic properties of other alternatives, namely natural dyes from plant and DSSCs. DSSC performances concerning transparent con- animal pigments (i.e. chlorophyll and porphyrin). ducting oxide substrates—indium-doped tin oxide (ITO) In this study, dyes extracted from natural native plants and fluorine-doped tin oxide (FTO)—led to significant dif- are used (Allium cepa L., Malva verticillata and Oregano) for ferences in internal global efficiency: from 2.24% for ITO TiO -DSSCs, yielding the highest efficiency of 0.54% [7]. to 9.6% for FTO [16]. TiO, titanium (IV) oxide and titania Golshan et al. used dye extracts from three marine plants can be used in applications involving the production of (Sar, Gar and Ent) and two terrestrial plants (Mav and Sua) DSSCs [17]. and reached the highest energy-conversion efficiency of Varying phases of crystalline TiO have different band 1.702% [8]. In other research, the plant-based dyes from gaps as compared to those of rutile TiO (3.0 eV). Anatase leaves used for DSSCs are red amaranth leaf shades [9], TiO of 3.2 eV determines the photocatalytic performance Epipremnum aureum plant leaf dyes [10] and peonidin-3- of TiO [18]. The mesoporous TiO layer provides a surface 2 2 glucoside (P3G) Acalypha godseffiana [11]. cps/eV Absorbance, a.u Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 435 for dye adsorption and an extensive reaction site for light A vacuum pump with a pressure of 0.2 bar absolute would absorption, leading to dye-regeneration efficiency and pull the liquid through the filter paper faster than the increasing the light-harvesting efficiency of DSSCs [16, 19]. gravity-separation method. These conditions cause a high short-circuit current () to I The final chlorophyll was then tested at 663 and 645 nm sc be realized in DSSCs [20]. using a UV–VIS spectrophotometer (LGS 53, BEL Photonics). Titanium film has the first intense absorption peak, The spectrophotometric analysis of the extracted filtrate which appears at ~4 eV [21]. Research has shown that dye/ and the calculation of the chlorophyll concentration used TiO is capable of transferring and injecting electrons ef- the following equation [25]: fectively [22]. Total chlorophyll content =(20.31 xA645 nm)+ Meanwhile, this research focuses on modifying the DSSC (8.05 xA663 nm) component to increase the power-conversion efficiency. (1) The novelty of this modification is achieved by making a The highest total chlorophyll was SP-Green, which was dye from the chlorophyll of Syzygium paniculatum leaves 88.750 mg/L. with leaf-colour variations. What is interesting about this plant is that the leaves have two colours: red and green. The content of red shoot leaves (Syzyginiumoleana) consists 1.2 Preparation of the TiO2-PEG paste of phenolics, flavonoid antioxidants and batulinic acid, as TiO powder was put into a beaker by adding PEG solution well as a new source of batulinic acid [23]. It is expected that at a ratio of 1:4. The paste-making process entailed heating flavonoid pigments from S. paniculatum plant leaves will be the mixture on a hotplate for 10 minutes at 65 C. suitable for use as a sensitizer for DSSC-based solar cells. The acid content makes the electron diffusion coefficient larger than in neutral conditions, so the electron-injection 1.3 Preparation of the TiO2-PEG coating using a rate is more significant [24]. Therefore, the present study spray gun attempts to develop a dye from S. paniculatum leaves to in- A spray gun was used for the process of coating TiO -PEG vestigate the optimal DSSC performance level with three pastes onto FTO glass. The spray gun had previously been leaf-colour variations. sterilized using ethanol to remove impurities. TiO -PEG paste was sprayed evenly on the surface of the 1  × 1  cm FTO glass. A  spray-gun pressure of 0.18  MPa was used so 1 Materials and methods that the TiO-PEG paste adhered to the FTO glass. They In this research, the material for the solar cell was obtained were then heated to a temperature of 200 C for 30 min- from S.  paniculatum plants grown in Bandung, Indonesia. utes. During this stage, the storage area had to be level to For the electrodes, FTO conductive glass sheet resistance ensure that the TiO solution remained even across the en- (Green Technology Company, China) with a value of <17  Ω/ tire surface. sq was prepared. Ethanol 96% and PEG (polyethylene glycol) were purchased from PT Brataco, whereas chloroform and TiO nanopowder were purchased from Agro Chemindo. 1.4 Dye-coated FTO immersion Scientific-grade potassium iodide (KI) was obtained from Immersion of the 1 x 1 cm FTO-TiO -PEG using chlorophyll the Kimia Lab. The last material, iodine crystal (I ), was from S. paniculatum was carried out in a glass beaker. The purchased from PT Dwilab Mandiri Scientific. The various immersion time was 3 hours in a closed room, after which stages of the methodology are described in the following it was taken out and allowed to dry. This process was suit- sections. able for both red leaves and green–red blends. 1.1 Syzygium paniculatum leaf extraction 1.5 Making carbon electrodes The extraction process for S.  paniculatum plants was Making a counter electrode required burning one side of done in the following order. First, the leaves were refined the FTO by shaking the FTO over a candle flame until the (blended until smooth) as 50 g + 50 ml aquadest. Distilled carbon was evenly distributed. The burning method lasted water, chloroform and 96% ethanol were then added to the for 50 seconds. Carbon adhered to the FTO glass with the smoothened leaves at a ratio of 3:2:1. After this, the solu- exact dimensions as FTO for the TiO-PEG coating. tion was refluxed for 10 minutes at 60 C and macerated 2 for 12 hours at ambient temperature in dark conditions. The resulting solution was separated using a vacuum 1.6 Preparation of the electrolyte solutions pump for an hour to gain the chlorophyll extraction used for the dye. A vacuum pump was connected to a hose and The electrolyte solution was prepared using 1 g of potas- a buffer flask. The chlorophyll mixture and solvent solu- sium iodide + 0.13  g of iodine (I ) [26] and dissolving in tion were poured through filter paper in a Buchner funnel. 100 ml of PEG. The solution was stirred with a stirring stick Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 436 | Clean Energy, 2021, Vol. 5, No. 3 until the iodine dissolved. The finished electrolyte solution where I is the short-circuit current, I is the optimal sc opt was stored in a dark bottle using a layer of aluminium foil. photostream,V is the open-circuit voltage, V is the op- oc opt The function of the electrolyte solution was to transport timal photovoltage and P is the input power of an incan- in –7 2 electrons from the carbon to the dye. descent lamp (279 lux or 408.456 × 10 W/cm ). Anthocyanins are coloured compounds responsible for most of the red, blue and purple colours in veget- 1.7 FTO assembly ables and ornamental plants that are members of the fla- The DSSC series was attached to the FTO glass with a vonoid pigment group. Fig. 2 shows the structure of the TiO -dye layer and an FTO glass counter electrode with a flavonoid pigment or dimethyl cardamonin (DMC) of the sandwich-layered structure as shown in Fig. 1 [27]. For elec- S. paniculatum [29]. trolyte contacts, on each end, an offset of 1 cm was given. Insulating-material spacers between the two electrodes were added to prevent quick contact. Before assembling, 3 Results and discussion one drop of the electrolyte solution was applied over the 3.1 Dye absorbance TiO layer. The layered structure was then clamped so that This research succeeded in synthesizing natural pigments the design became tighter and did not move easily. from S. paniculatum plant leaves using only distilled water, ethanol and chloroform, at a ratio of 3:2:1. Fig. 3 shows the 2 Characterization and measurement absorption of natural dyes of the S. paniculatum plant with various leaf colours. The LGS 53 UV–VIS spectrometer (BEL Photonics) showed The maximum absorbance spectrum of the S. paniculatum that the absorption spectrum of the extract was from wave- leaf pigments in this study was at a wavelength of 663 nm. length 663  nm to wavelength 645  nm. Observation of the Our results are consistent with those of other studies that FTO-TiO /PEG-dye was carried out using the SEM Oxford in- have used anthocyanin flavonoid pigments as dye sensi- strument (Aztec LIVE). The DSSC photoelectric test used an tizers, reporting maximum absorbance in the 600- to 680- incandescent light photon source at room temperature. The nm region [30, 31]. The S. paniculatum spectrum at 663 nm is cable to both parts of the DSSC surface had an active area of 2 in the 600- to 680-nm range indicated for flavonoids. 1 × 1 cm . The FTO-TiO /PEG-dye part was the positive pole, Chlorophyll using ethanol solution had three peaks: where the electrons came out first through the side. This at 436, 470 and 664  nm [32–34]. The maximum absorb- part was also the side exposed to light as a light absorber. ance spectrum of the SP-Green results for the flavonoid The other side (the FTO side with the carbon layer) was the negative side, where the electrons would come back. The O3A electricity that came out of the DSSC was direct current (DC) O4A so that the multimeter regulated DC and voltage. The re- C18A C5A C9A C7A C11A sults of this test were the and I V  values. sc sc C10A C6A C8A C4A C12A The equations for calculating the charging factor (FF) and solar cell efficiency (η) were as follows [28]: C1A (I × V ) C3A C13A O1A opt opt C15A FF = × 100% (2) C14A O2A C2A (I × V ) sc oc C16A C17A (FF × I × V ) sc oc (3) η = × 100% in Fig. 2: Flavonoid structure of the Syzygium paniculatum plant dye 3.5 SP-Red T O -PEG i 2 SP-Green 2.5 – SP-Mix F F 1.5 T T O O 0.5 eletrolyte 300 400 500 600 700 800 Carbon Wavelength, nm Fig. 3: The relationship between wavelength and absorbance of natural Fig. 1: Schematic diagram of the DSSC assembly dyes from Syzygium paniculatum of various leaf colours Absorbance, a.u Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 437 pigments and chlorophyll pigment in this study had a high scanning electron microscope (FESEM) (AZtecLIVE, Oxford value, with a maximum absorbance of 3.13 a.u. The intense Instruments) and EDX analysis. interaction between cyanide-glycosides in flavonoid pig- However, the three of them formed agglomerated and ments causes an increase in the absorbance value of the aggregated nanoparticles with an irregular shape. The ten- dye pigment. The intensity, position and shape of stains dency of the particles to agglomerate was directly related that dissolve in different solvents can change [35]. to the increase in crystal size obtained. The EDX spectrum The cause of this condition is the interaction between dis- confirms that the sample consists of O, Si, Na, Ti, K, Ca, Mg, solved molecules, solvent-dissolved interactions and the nature Al and I. Atoms containing the atomic ratio of O to Ti, within of the polarity of the solution in the form of the hydrogen–OH the resolution limit (approximately ± one atomic%), ap- bond. The leaves of the S.  paniculatum plant, which contain proach 3.47:1 (SP-Red), 4.58:1 (SP-Green) and 2.98:1 (SP-Mix). flavonoid pigments, have a high absorption capacity making These values were above the required stoichiometric them suitable for DSSC-based solar cell sensitizers. ratio of TiO, which was 2:1. This condition occurred be- The higher the ability of the pigment to absorb photons, cause of the addition of O elements from PEG (CH + 2O 2n 4n n the better the performance of the DSSC-based solar cells; + 1) and chlorophyll (chlorophyll a, namely C H O N Mg, 55 72 5 4 DSSC-based solar cells with stains or dyes function as a and chlorophyll b, namely C H O N Mg). The Si, Na, Mg 55 70 6 4 photon absorber from sunlight. The more photon energy and Al elements came from chlorophyll nutrient elements, absorbed, the higher the voltage value is. The results of ab- while K and I came from electrolytes made from a mixture sorbing flavonoid pigments in this study are of high import- of KI and I . Furthermore, the EDX results revealed the Mg ance in the visible spectrum so that they can develop natural content for SP-Green and SP-Mix. It did not exist for SP-Red sensitizing dye-based solar cells. The dye-absorption spec- because the chlorophyll in red leaves was unstable due to trum and adherence to the semiconductor surface of TiO are the influence of light, temperature and oxygen, so it effi- essential factors in determining the efficiency of DSSCs [36]. ciently degraded, resulting in loss of Mg. The peak area detected was elemental Ti at 5  keV for FTO-TiO with all three dyes and Zn at 9.6 keV for FTO-TiO 2 2 3.2 Morphology of FTO-TiO2/PEG-dye coating with SP-Red. The results of this study are consistent with dye absorbance studies that have reported detecting elemental Ti at 5 keV Figs 4–6 show the results of surface morphological obser - (better than the Hummer enhancement method) [37], i.e. vations of the FTO-TiO/PEG-dye coating using an emission with Ti showing a value of 4.5 keV [38]. AB Spectrum Spectrum Spectrum 4 Ti Ti Zn Al Si K K I II Ti Zn Zn 0 123456789 keV Fig. 4: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for red leaves cps/eV Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 438 | Clean Energy, 2021, Vol. 5, No. 3 A B Spectrum Spectrum Spectrum Na Ca Mg Si Ti Al K Ca ll Ti Ti 0 12345678 9 keV Fig. 5: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for green leaves A B Spectrum Spectrum Spectrum Ti Ti Ca Mg Si K Ti Ca l 0 12345678 9 keV Fig. 6: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for green–red mixed leaves cps/eV cps/eV Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 439 Table 1: FF value and DSSC performance 2 2 FTO-TiO / PEG-dye pH I (mA/cm ) V (V) I (mA/cm ) V (V) FF (%) η (%) 2 sc sc max max SP-Red 2 0.0039 0.258 0.003 0.15 44.723 1.102 SP-Green 5.5 0.0047 0.432 0.0039 0.39 74.911 3.724 SP-Green (deviation) 5.5 0.0025 0.334 0.0027 0.21 67.904 1.388 SP-Mix 4 0.0048 0.323 0.0039 0.25 62.887 2.387 SP-Green has high Mg content and can interact strongly 3.3 Photovoltaic performance in DSSCs with TiO . By composting it with porphyrin and using it Eighteen experiments on the DSSC photovoltaic perform- for mesoporous TiO , it is hoped that it can increase the ance were carried out in this studyT. able 1 shows only efficiency of DSSC. the best results with one data deviation. The results show that the solar cells have succeeded in converting light en- ergy into electricity. Dye or dye using S. paniculatum leaves Funding seemed to affect the performance of the DSSC. DSSC testing produced voltages and currents with different variations. This research was funded by the UPPM- Politeknik Negeri Bandung in the context of competitiveness between groups in the field of Meanwhile, when the solar cell was without light illumin- expertise. ation, there was no voltage measured on the solar cell. It was found that FTO-TiO/PEG-dye using SP-Green has the highest efficiency (3.724%) because green leaves have stable chlorophyll. 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The performance of solar cells using chlorophyll dye from Syzygium paniculatum

Clean Energy , Volume 5 (3) – Sep 1, 2021

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Copyright © 2021 National Institute of Clean-and-Low-Carbon Energy
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10.1093/ce/zkab022
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Abstract

3.5 SP-Red SP-Green 2.5 SP-Mix DSSC Process 1.5 0.5 300 400 500 600 700 800 Wavelength, nm FTO with TiO + PEG The relationship between wavelength and absorbance coating uses a 0.18 MPa spray gun Spectrum Ti Ti Counter electrode Ca Mg Si K Ca l Ti from carbon 0 0 123456789 keV EDX test result FTO-TiO / I V (V)V I (V) FF 2 sc SC max max –2 –2 PEG- Dye (mA.cm ) (mA.cm ) (%)(%) SP-Red 0.0039 0.258 0.003 0.15 44.723 1.102 DSSC (Electrode + Electrolyte + Counter SP-Green 0.0047 0.432 0.0039 0.39 74.911 3.724 electrode) SP-Mix 0.0048 0.323 0.0039 0.25 62.887 2.387 FF value and DSSC performance Keywords: chlorophyll; flavonoids; photoanode TiO ; solar cell; Syzygium paniculatum Further, the porphyrin dyes were evaluated as the sen- Introduction sitizers of DSSCs based on an I/I electrolyte, increasing 2 3 Dye-sensitized solar cell (DSSC) technology is a third- efficiency dramatically to 11.5% [12]. Making DSSC (XW28) generation dye-based solar cell technology with easy fabri- using porphyrin dye by inserting a chain into its appro- cation, low production costs and environmentally friendly priate position of the benzothiadiazolyl acceptor section [1–5] silicon-based solar cells. However, silicon-based solar resulted in a high efficiency of 10.14% [13]. Higashino re- cells have several disadvantages: pure silicon, high tech- viewed research using porphyrin dyes to increase effi- nology, dangerous chemicals and high prices. Therefore, ciency by ≤13% [14]. Development of a synthetic organic researchers are interested in developing DSSCs. The dyes dye Z2 linked to a double-bond porphyrin dye and added used today are synthetic dyes and natural dyes. Synthetic with chenodeoxycholic acid (CDCA), XW61 provided 12.4% dyes such as the ruthenium complex contain heavy metals efficiency [15]. that are less favourable in the environment [6]. Due to such Moreover, solar cells with TiO material are essen- difficult and expensive designation, researchers look for tial factors that determine the photovoltaic properties of other alternatives, namely natural dyes from plant and DSSCs. DSSC performances concerning transparent con- animal pigments (i.e. chlorophyll and porphyrin). ducting oxide substrates—indium-doped tin oxide (ITO) In this study, dyes extracted from natural native plants and fluorine-doped tin oxide (FTO)—led to significant dif- are used (Allium cepa L., Malva verticillata and Oregano) for ferences in internal global efficiency: from 2.24% for ITO TiO -DSSCs, yielding the highest efficiency of 0.54% [7]. to 9.6% for FTO [16]. TiO, titanium (IV) oxide and titania Golshan et al. used dye extracts from three marine plants can be used in applications involving the production of (Sar, Gar and Ent) and two terrestrial plants (Mav and Sua) DSSCs [17]. and reached the highest energy-conversion efficiency of Varying phases of crystalline TiO have different band 1.702% [8]. In other research, the plant-based dyes from gaps as compared to those of rutile TiO (3.0 eV). Anatase leaves used for DSSCs are red amaranth leaf shades [9], TiO of 3.2 eV determines the photocatalytic performance Epipremnum aureum plant leaf dyes [10] and peonidin-3- of TiO [18]. The mesoporous TiO layer provides a surface 2 2 glucoside (P3G) Acalypha godseffiana [11]. cps/eV Absorbance, a.u Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 435 for dye adsorption and an extensive reaction site for light A vacuum pump with a pressure of 0.2 bar absolute would absorption, leading to dye-regeneration efficiency and pull the liquid through the filter paper faster than the increasing the light-harvesting efficiency of DSSCs [16, 19]. gravity-separation method. These conditions cause a high short-circuit current () to I The final chlorophyll was then tested at 663 and 645 nm sc be realized in DSSCs [20]. using a UV–VIS spectrophotometer (LGS 53, BEL Photonics). Titanium film has the first intense absorption peak, The spectrophotometric analysis of the extracted filtrate which appears at ~4 eV [21]. Research has shown that dye/ and the calculation of the chlorophyll concentration used TiO is capable of transferring and injecting electrons ef- the following equation [25]: fectively [22]. Total chlorophyll content =(20.31 xA645 nm)+ Meanwhile, this research focuses on modifying the DSSC (8.05 xA663 nm) component to increase the power-conversion efficiency. (1) The novelty of this modification is achieved by making a The highest total chlorophyll was SP-Green, which was dye from the chlorophyll of Syzygium paniculatum leaves 88.750 mg/L. with leaf-colour variations. What is interesting about this plant is that the leaves have two colours: red and green. The content of red shoot leaves (Syzyginiumoleana) consists 1.2 Preparation of the TiO2-PEG paste of phenolics, flavonoid antioxidants and batulinic acid, as TiO powder was put into a beaker by adding PEG solution well as a new source of batulinic acid [23]. It is expected that at a ratio of 1:4. The paste-making process entailed heating flavonoid pigments from S. paniculatum plant leaves will be the mixture on a hotplate for 10 minutes at 65 C. suitable for use as a sensitizer for DSSC-based solar cells. The acid content makes the electron diffusion coefficient larger than in neutral conditions, so the electron-injection 1.3 Preparation of the TiO2-PEG coating using a rate is more significant [24]. Therefore, the present study spray gun attempts to develop a dye from S. paniculatum leaves to in- A spray gun was used for the process of coating TiO -PEG vestigate the optimal DSSC performance level with three pastes onto FTO glass. The spray gun had previously been leaf-colour variations. sterilized using ethanol to remove impurities. TiO -PEG paste was sprayed evenly on the surface of the 1  × 1  cm FTO glass. A  spray-gun pressure of 0.18  MPa was used so 1 Materials and methods that the TiO-PEG paste adhered to the FTO glass. They In this research, the material for the solar cell was obtained were then heated to a temperature of 200 C for 30 min- from S.  paniculatum plants grown in Bandung, Indonesia. utes. During this stage, the storage area had to be level to For the electrodes, FTO conductive glass sheet resistance ensure that the TiO solution remained even across the en- (Green Technology Company, China) with a value of <17  Ω/ tire surface. sq was prepared. Ethanol 96% and PEG (polyethylene glycol) were purchased from PT Brataco, whereas chloroform and TiO nanopowder were purchased from Agro Chemindo. 1.4 Dye-coated FTO immersion Scientific-grade potassium iodide (KI) was obtained from Immersion of the 1 x 1 cm FTO-TiO -PEG using chlorophyll the Kimia Lab. The last material, iodine crystal (I ), was from S. paniculatum was carried out in a glass beaker. The purchased from PT Dwilab Mandiri Scientific. The various immersion time was 3 hours in a closed room, after which stages of the methodology are described in the following it was taken out and allowed to dry. This process was suit- sections. able for both red leaves and green–red blends. 1.1 Syzygium paniculatum leaf extraction 1.5 Making carbon electrodes The extraction process for S.  paniculatum plants was Making a counter electrode required burning one side of done in the following order. First, the leaves were refined the FTO by shaking the FTO over a candle flame until the (blended until smooth) as 50 g + 50 ml aquadest. Distilled carbon was evenly distributed. The burning method lasted water, chloroform and 96% ethanol were then added to the for 50 seconds. Carbon adhered to the FTO glass with the smoothened leaves at a ratio of 3:2:1. After this, the solu- exact dimensions as FTO for the TiO-PEG coating. tion was refluxed for 10 minutes at 60 C and macerated 2 for 12 hours at ambient temperature in dark conditions. The resulting solution was separated using a vacuum 1.6 Preparation of the electrolyte solutions pump for an hour to gain the chlorophyll extraction used for the dye. A vacuum pump was connected to a hose and The electrolyte solution was prepared using 1 g of potas- a buffer flask. The chlorophyll mixture and solvent solu- sium iodide + 0.13  g of iodine (I ) [26] and dissolving in tion were poured through filter paper in a Buchner funnel. 100 ml of PEG. The solution was stirred with a stirring stick Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 436 | Clean Energy, 2021, Vol. 5, No. 3 until the iodine dissolved. The finished electrolyte solution where I is the short-circuit current, I is the optimal sc opt was stored in a dark bottle using a layer of aluminium foil. photostream,V is the open-circuit voltage, V is the op- oc opt The function of the electrolyte solution was to transport timal photovoltage and P is the input power of an incan- in –7 2 electrons from the carbon to the dye. descent lamp (279 lux or 408.456 × 10 W/cm ). Anthocyanins are coloured compounds responsible for most of the red, blue and purple colours in veget- 1.7 FTO assembly ables and ornamental plants that are members of the fla- The DSSC series was attached to the FTO glass with a vonoid pigment group. Fig. 2 shows the structure of the TiO -dye layer and an FTO glass counter electrode with a flavonoid pigment or dimethyl cardamonin (DMC) of the sandwich-layered structure as shown in Fig. 1 [27]. For elec- S. paniculatum [29]. trolyte contacts, on each end, an offset of 1 cm was given. Insulating-material spacers between the two electrodes were added to prevent quick contact. Before assembling, 3 Results and discussion one drop of the electrolyte solution was applied over the 3.1 Dye absorbance TiO layer. The layered structure was then clamped so that This research succeeded in synthesizing natural pigments the design became tighter and did not move easily. from S. paniculatum plant leaves using only distilled water, ethanol and chloroform, at a ratio of 3:2:1. Fig. 3 shows the 2 Characterization and measurement absorption of natural dyes of the S. paniculatum plant with various leaf colours. The LGS 53 UV–VIS spectrometer (BEL Photonics) showed The maximum absorbance spectrum of the S. paniculatum that the absorption spectrum of the extract was from wave- leaf pigments in this study was at a wavelength of 663 nm. length 663  nm to wavelength 645  nm. Observation of the Our results are consistent with those of other studies that FTO-TiO /PEG-dye was carried out using the SEM Oxford in- have used anthocyanin flavonoid pigments as dye sensi- strument (Aztec LIVE). The DSSC photoelectric test used an tizers, reporting maximum absorbance in the 600- to 680- incandescent light photon source at room temperature. The nm region [30, 31]. The S. paniculatum spectrum at 663 nm is cable to both parts of the DSSC surface had an active area of 2 in the 600- to 680-nm range indicated for flavonoids. 1 × 1 cm . The FTO-TiO /PEG-dye part was the positive pole, Chlorophyll using ethanol solution had three peaks: where the electrons came out first through the side. This at 436, 470 and 664  nm [32–34]. The maximum absorb- part was also the side exposed to light as a light absorber. ance spectrum of the SP-Green results for the flavonoid The other side (the FTO side with the carbon layer) was the negative side, where the electrons would come back. The O3A electricity that came out of the DSSC was direct current (DC) O4A so that the multimeter regulated DC and voltage. The re- C18A C5A C9A C7A C11A sults of this test were the and I V  values. sc sc C10A C6A C8A C4A C12A The equations for calculating the charging factor (FF) and solar cell efficiency (η) were as follows [28]: C1A (I × V ) C3A C13A O1A opt opt C15A FF = × 100% (2) C14A O2A C2A (I × V ) sc oc C16A C17A (FF × I × V ) sc oc (3) η = × 100% in Fig. 2: Flavonoid structure of the Syzygium paniculatum plant dye 3.5 SP-Red T O -PEG i 2 SP-Green 2.5 – SP-Mix F F 1.5 T T O O 0.5 eletrolyte 300 400 500 600 700 800 Carbon Wavelength, nm Fig. 3: The relationship between wavelength and absorbance of natural Fig. 1: Schematic diagram of the DSSC assembly dyes from Syzygium paniculatum of various leaf colours Absorbance, a.u Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 437 pigments and chlorophyll pigment in this study had a high scanning electron microscope (FESEM) (AZtecLIVE, Oxford value, with a maximum absorbance of 3.13 a.u. The intense Instruments) and EDX analysis. interaction between cyanide-glycosides in flavonoid pig- However, the three of them formed agglomerated and ments causes an increase in the absorbance value of the aggregated nanoparticles with an irregular shape. The ten- dye pigment. The intensity, position and shape of stains dency of the particles to agglomerate was directly related that dissolve in different solvents can change [35]. to the increase in crystal size obtained. The EDX spectrum The cause of this condition is the interaction between dis- confirms that the sample consists of O, Si, Na, Ti, K, Ca, Mg, solved molecules, solvent-dissolved interactions and the nature Al and I. Atoms containing the atomic ratio of O to Ti, within of the polarity of the solution in the form of the hydrogen–OH the resolution limit (approximately ± one atomic%), ap- bond. The leaves of the S.  paniculatum plant, which contain proach 3.47:1 (SP-Red), 4.58:1 (SP-Green) and 2.98:1 (SP-Mix). flavonoid pigments, have a high absorption capacity making These values were above the required stoichiometric them suitable for DSSC-based solar cell sensitizers. ratio of TiO, which was 2:1. This condition occurred be- The higher the ability of the pigment to absorb photons, cause of the addition of O elements from PEG (CH + 2O 2n 4n n the better the performance of the DSSC-based solar cells; + 1) and chlorophyll (chlorophyll a, namely C H O N Mg, 55 72 5 4 DSSC-based solar cells with stains or dyes function as a and chlorophyll b, namely C H O N Mg). The Si, Na, Mg 55 70 6 4 photon absorber from sunlight. The more photon energy and Al elements came from chlorophyll nutrient elements, absorbed, the higher the voltage value is. The results of ab- while K and I came from electrolytes made from a mixture sorbing flavonoid pigments in this study are of high import- of KI and I . Furthermore, the EDX results revealed the Mg ance in the visible spectrum so that they can develop natural content for SP-Green and SP-Mix. It did not exist for SP-Red sensitizing dye-based solar cells. The dye-absorption spec- because the chlorophyll in red leaves was unstable due to trum and adherence to the semiconductor surface of TiO are the influence of light, temperature and oxygen, so it effi- essential factors in determining the efficiency of DSSCs [36]. ciently degraded, resulting in loss of Mg. The peak area detected was elemental Ti at 5  keV for FTO-TiO with all three dyes and Zn at 9.6 keV for FTO-TiO 2 2 3.2 Morphology of FTO-TiO2/PEG-dye coating with SP-Red. The results of this study are consistent with dye absorbance studies that have reported detecting elemental Ti at 5 keV Figs 4–6 show the results of surface morphological obser - (better than the Hummer enhancement method) [37], i.e. vations of the FTO-TiO/PEG-dye coating using an emission with Ti showing a value of 4.5 keV [38]. AB Spectrum Spectrum Spectrum 4 Ti Ti Zn Al Si K K I II Ti Zn Zn 0 123456789 keV Fig. 4: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for red leaves cps/eV Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 438 | Clean Energy, 2021, Vol. 5, No. 3 A B Spectrum Spectrum Spectrum Na Ca Mg Si Ti Al K Ca ll Ti Ti 0 12345678 9 keV Fig. 5: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for green leaves A B Spectrum Spectrum Spectrum Ti Ti Ca Mg Si K Ti Ca l 0 12345678 9 keV Fig. 6: FESEM of (a) electron image, (b) EDX layered image, (c) EDX spectrum and (d) element-composition data for green–red mixed leaves cps/eV cps/eV Downloaded from https://academic.oup.com/ce/article/5/3/433/6333455 by DeepDyve user on 03 August 2021 Sri Wuryanti | 439 Table 1: FF value and DSSC performance 2 2 FTO-TiO / PEG-dye pH I (mA/cm ) V (V) I (mA/cm ) V (V) FF (%) η (%) 2 sc sc max max SP-Red 2 0.0039 0.258 0.003 0.15 44.723 1.102 SP-Green 5.5 0.0047 0.432 0.0039 0.39 74.911 3.724 SP-Green (deviation) 5.5 0.0025 0.334 0.0027 0.21 67.904 1.388 SP-Mix 4 0.0048 0.323 0.0039 0.25 62.887 2.387 SP-Green has high Mg content and can interact strongly 3.3 Photovoltaic performance in DSSCs with TiO . By composting it with porphyrin and using it Eighteen experiments on the DSSC photovoltaic perform- for mesoporous TiO , it is hoped that it can increase the ance were carried out in this studyT. able 1 shows only efficiency of DSSC. the best results with one data deviation. The results show that the solar cells have succeeded in converting light en- ergy into electricity. Dye or dye using S. paniculatum leaves Funding seemed to affect the performance of the DSSC. DSSC testing produced voltages and currents with different variations. This research was funded by the UPPM- Politeknik Negeri Bandung in the context of competitiveness between groups in the field of Meanwhile, when the solar cell was without light illumin- expertise. ation, there was no voltage measured on the solar cell. It was found that FTO-TiO/PEG-dye using SP-Green has the highest efficiency (3.724%) because green leaves have stable chlorophyll. 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Clean EnergyOxford University Press

Published: Sep 1, 2021

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