Advancement in Photogalvanic Cell for Solar Energy Harvesting: A Review

Abstract

The Photogalvanic effect is a promising mechanism for the conversion of solar energy into electrical energy, utilizing a variety of chemical systems to enhance efficiency and storage capacity. The operation of Photogalvanic cells is characterized by the absorption of solar energy by a photosensitizer, which generates energy-rich species in an electrolyte solution. This process creates a Photopotential between two electrodes, enabling the production of electricity without the need for complex semiconductor materials found in conventional solar cells. About 196 research articles on the development of Photogalvanic cell we have been reviewed here. With comparison of 87 system, the electric parameters of the cell containing single dye, mixed dye and natural dye with reductant and surfactant have presented in tabular form (Table-1). We have also focus on the challenges limitation, future aspect in field of photochemical conversion of solar energy and its storage. This review explores the recent advancements in Photogalvanic cells, devices that convert light energy into electrical energy via photochemical processes. It highlights innovations in materials, the mechanisms of charge generation and transfer, challenges in efficiency and stability, and the diverse applications of Photogalvanic cells, in sustainable energy production. The paper also discusses future trends and emerging technologies that could shape the development of Photogalvanic cells, positioning them as a promising technology in the renewable energy landscape.

Introduction

I. INTRODUCTION

Solar energy is a form of renewable energy. It is created when the sun undergoes nuclear fusion. In 1.5 days, the sun generates 1.7 x 1022 J of energy. This energy is equivalent to the total energy contained in the world's 3 trillion barrels of oil reserves. Humans use 4.6 x 1020 J of energy each year. The sun produced this amount of energy in one hour.[1] Solar energy is a low-cost, easily available, and environmentally friendly source of energy that has the potential to produce almost no emissions.[2]

People have been using sun energy since the 17th century BCE. Ancient civilizations (Rome and Greece) displayed the first documented use of sunlight by lighting torches with mirrors for religious purposes, and ancient buildings employed passive solar design, which entails harnessing sunlight to heat and light inside spaces. A.E. Becquerel discovered the outstanding and revolutionary Becquerel effect in 1839. The photoelectric effect was discovered in the 20th century by Einstein and other scientists. This encouraged research into materials whose chemical composition would enable them to be used to generate electrical energy from solar radiation.[3] Solar energy is directly converted into solar power via solar cells, which are based on the photovoltaic effect. Solar cells can be made with a single layer of light-absorbing material (single-junction) or in a variety of physical configurations (multi-junctions) to take advantage of varied absorption and charge separation methods.[4] Solar cells includes, silicon solar cells, thin-film solar cells, perovskite solar cells, quantum dot cells, organic solar cells, dye-sensitized solar cells, photogalvanic cells.  Photogalvanic cells are electrochemical devices, that use dye-sensitized solutions to convert and store solar radiation through the “Photogalvanic Effect.” Rideal and Williams discovered it[5], while Rabinowitch conducted an extensive investigation and firstly used the word.[6], [7] Furthermore, several research groups, including Waber and Matijevic[8], Kamat and Lichtin[9], [10], Albery and Foulds[11], etc., have examined this effect on various systems of photogalvanic cells for solar power conversion and storage.

II. COMPONENTS OF PHOTOGALVANIC CELLS (PG CELLS)

The fundamental elements of PG cells are electrolytes, electrodes, assembly setup, and a light source.

A. Electrolytes

The electrolyte facilitates the movement of ions between the two electrodes in the photogalvanic cell. The electrolyte helps to stabilize the photogalvanic cell by maintaining the proper ionic conditions necessary for continuous operation. A well-chosen electrolyte can enhance the conversion of solar energy into electrical energy and improve the cell's longevity.

Photogalvanic cells containing dye/photosensitizer, reductant, surfactant, and acid/alkali are important electrolytes component for storage and low-cost assembly setup.

1. Photosensitizer: Dyes/photosensitizers are essential to the operation of photogalvanic cells because they absorb solar light and start the processes that lead to electron transfer. So, photosensitizer should be photostable and good light-harvesting material. Photochemical reactions require a specific concentration of the dye. Light and dye molecules are both particles in nature and interact according to Stark-Einstein's law, a lower concentration of photosensitizer led to a decrease in photopotential and photocurrent because there were fewer photosensitizer molecules available for excitation and subsequent electron donation to the platinum electrode. Similarly, at larger concentrations, a large amount of the light is absorbed by dye molecules because photogalvanic cells are diffusion-controlled. Increased concentration may also result in faster recombination between injected electrons and dye. Hence, when photosensitizer concentration rises, photopotential and photocurrent are increased until they reach their highest values and further decrease.[3] Dyes are classified into synthetic and natural dyes. Natural dyes consist of complex blends of components sourced from natural materials like plants, animals, or minerals. Synthetic dyes are produced in a lab. Chemicals are produced to create synthetic dyes. Thionine dye was mostly used as a primary electrolyte until around the 1980s.[6], [7], [8], [10] Later on, a variety of dyes from various classes were tested in photogalvanic cells as photosensitizers like Malachite Green[12], Congo red[13], Rose Bengal[14], Quinoline Yellow[15], Alizarine Red S[16], etc. Dube[17] used a mixed dye system (Azur A, Azur B, and Azur C with mannitol and NTA) in photogalvanic cells to improve conversion efficiency and also discovered that the dyes increased the ability of solution to absorb solar energy, which led to a larger area of light absorption. Later, a variety of mixed dye systems of the photogalvanic cells have been explored, including Toluidine Blue + Brilliant Cresyl Blue[18], Brilliant Green + Celestine Blue[19], Naphthol Green B + Janus Green B[20], Xylene Cyanol FF + Patent Blue[21], Sudan Black- B + Azur-B[22], etc. Synthetic dyes exhibit high conversion efficiency and superior chemical stability, rendering them among the top sensitizers; however, they tend to be quite costly and hazardous. Also, using artificial dye sensitizers goes against the main goals of solar energy harvesting's sustainability and renewable nature. Consequently, numerous, researchers have turned to natural dyes because of their wide range of possibilities, due to their completely biodegradability, inexpensive, non-toxic, and readily available, they can be utilized for the same application. Natural dyes are present in different parts of plants like leaves, flowers, fruits, and seeds which are obtained with easy methods. Many natural dyes derived from plant sources have been used as photosensitizers in photogalvanic cells for solar energy harvesting showed in Table - 1.
2. Reductant: In the first systematic photogalvanic cell, iron salt was used as an electron donor. However, the photocurrent and photopotential were low due to recombination and dissipation of free energy into heat. In 1958, W. Hendrich[23] used ascorbic acid as an irreversible reductant, which was easily soluble in dyes and faster for redox transfer, enhancing conversion efficiency. Albery et al.[24] proved that irreversible reducing agents are more beneficial than reversible ones in photogalvanic cells. Several irreversible reductants have been used as electrolytes like EDTA, triethylamine, triethanolamine[25], hydroquinone[26], ascorbic acid[27], [28], oxalic acid[29], fructose[30], etc, and mixed reductants mannitol-nitrilotriacetic acid[31], EDTA with oxalic acid, nitrilotriacetic acid, and dextrose, respectively[32], etc have been used to improve electrical output. Similar to the dye concentration, the reductant concentration also follows a similar trend. Lower reductant concentrations result in lower electrical output because fewer reductant molecules are available to donate electrons to photosensitizers, and higher reductant concentrations cause photopotential and photocurrent to fall because an excess of reductant molecules prevent dye molecules from reaching the electrode in the appropriate time.
3. Surfactant: Surfactants are chemical substances that are naturally amphiphilic. This implies that they include both water-soluble (hydrophilic) and water-insoluble (hydrophobic) groups. Surfactants are commonly used to inhibit the recombination reaction in photochemical processes. SLS was initially used by Zhi-Chu Bi[33] as a surfactant in a solution that contained thionine as a dye and Fe2+/Fe3+ as a reductant. It is interesting to observe that SLS surfactant solution is used in photogalvanic cells to dissolve thionine in water. In India, first of all, Srivastava et al.[34] used polyvinyl methyl ether as a surfactant to improve photogalvanic cell conversion efficiency. Valenty[35] investigated the interactions of functionalized surfactants monolayer films and discovered that methylene blue adsorption to photogalvanic electrodes is connected to the orientation and absorption spectra of its surfactant analogues. SLS is widely used as a surfactant in the photogalvanic cells.[36], [37] Other surfactants, such as Triton-X 100[14], Brij-35[38], DSS[22], CPC[39], Tergitol-7[40], CTAB[41], Tween 80[42], Benzalkonium Chloride[29], etc, and mixed surfactants such as NaLS+CTAB and NaLS+Tween-80[43], NaLS+CPC+Tween-80[44], Brij-35+NaLS[45], etc are being utilized to enhance the electrical output of photogalvanic cells. The use of surfactants has been found to improve cell stability and electrical output because surfactant molecules interact with dye through charge transfer or coulombic interaction, depending on the nature of the dye and surfactants. The cell is more stable in a cationic micelle medium (if the dye is anionic) than in an aqueous medium.[46] However, the conversion efficiency of systems with different surfactants is often found to be in the order anionic>non-ionic>cationic (if the dye is cationic).[47] When a surfactant and dye have opposite charges, a strong dye-surfactant complex forms in which the dye molecule is covered by surfactant micelles in a regular shape that inhibits intermolecular twisting and increases fluorescence.[48] Studies have shown that when surfactant concentration increased both the photo-potential and photo-current increased until they reached a maximum and subsequently decreased.
4. Alkali/acid: The conductivity of the cell is affected by the medium of the solution. An appropriate pH can increase the electrical output because pH affects the back reaction. Initially, several acids such as oxalic acid[49], H2SO4[50], HCl[51], and CH3COOH[52] were utilized to maintain the pH of electrolytes. Nowadays, alkali mediums such as NaOH[53], [54], [55], KOH[56] are used in the fabrication of the photogalvanic cells, because most of the photosensitizers/dyes are more soluble and stable in an alkali medium. It is commonly observed that, when the concentration of solution medium (pH) increases, the cell output of the regenerative photogalvanic cell also increases until it reaches a maximum and then decreases. The optimal pH is related to the pKa value of the reductant. The desired pH is greater than the pKa value (pH> pKa). This could be explained by the reductant being available in its anionic form, which is a better donor form.[57]

A. Electrode

The photogalvanic cell technique uses two electrodes: the working electrode (acting as the anode), which is exposed to light, and the counter electrode (acting as the cathode), which is kept in the dark chamber. The working electrode facilitates electron exchange between the semi/leuco reduced sensitizer molecule and the external circuit, while the counter electrode completes the circuit and conducts current.

Initially, researchers used both coated and uncoated Pt electrodes as the working electrode, but the electrical output obtained from both was low due to the large size of the platinum electrode.[6] Later on, small-sized Pt electrodes were used to improve the performance of photogalvanic cells.[58], [59], [60], [61] A platinum electrode is considered inert because platinum has a high ability to facilitate electron exchange. However, it is costly and not easily accessible in the local market, making its procurement expensive and time-consuming. Nowadays, different types of electrodes such as Cu, Cu-Zn alloy (brass)[62], Al, Cu-Ni alloy, Al-Mg alloy[63], etc., are used as working electrodes in PGCs. A saturated calomel electrode is usually used as a counter electrode or reference electrode but in recent times various types of reference electrodes such as graphite counter electrodes[64] have been used.

B. Light source

The electrical output of a cell is affected by the light source and its distance from the cell surface. Rabinowitch initially used a 1000 W lamp as the light source in the first thionine–iron photogalvanic cell.[6] Subsequently, various researchers used different light intensities, such as 900 W xenon lamp[65], 500 W xenon lamp[66], 450 W xenon lamp[67], 300 W[68], 250 W tungsten halogen lamp[69], 150 W xenon lamp[70], 100 W tungsten lamp[71], and 2 W Ar laser[72]. Nowadays, a 200 W tungsten lamp[19], [73], [74], [75] is used as the light source in PGCs. However, direct light is not useful because the radiation produces Infrared radiations that raise the temperature of the system. Therefore, filters are used for light filtration. Generally, water (flow) is used as a light filter[76], but in some systems, glass filters are also used[66]. Daul et al.[77] alternately illuminated the two electrodes and observed a very stable power output. Some scientists used other filters with water for light filtration, such as FeSO4 solution.[7], [8] However, water is mostly used as a filter in regular photogalvanic cell work nowadays. The distance between the light source and the cell surface is typically about 15 cm in recent work.[68]

As light intensity rises, more dye molecules are photoexcited and reduced by reductant due to the photogalvanic effect. This effect is correlated with the ratio of bleached and unbleached dye in the solution. Photocurrent and photopotential increase linearly and logarithmically with light intensity, respectively but the cell temperature also increases. In general, photogalvanic cells use 10.4mWcm-2 of light intensity[78], but at greater intensities (>150mWcm-2), the photogalvanic effect approaches a limit.[79]

C. Experimental Setup and Mechanism

The two electrodes used in the photogalvanic cell technique are the working electrode (often platinum, Pt) which is exposed to light, and the counter electrode (commonly a saturated calomel electrode, SCE) which is in the dark.

A solution of photosensitizer (photon-absorbing species), reductant (electron-donating species), and surfactant (efficiency enhancer agent) in an alkaline medium are used to fill the space between the electrodes. The net volume of electrolyte remains 25 ml. The working electrode in photogalvanic cells facilitates electron exchange between the semi/leuco-reduced sensitizer molecule and the external circuit. The circuit is completed with the help of the counter electrode, which also conducts current flow.[62] They are shown in the experimental setup (Fig -1).

D. Mechanisms

Illuminated Chamber- On illumination, a photon is absorbed by the dye, which gets excited. The excited form of the dye removes an electron from the reductant and converts into a semi or leuco form of the dye.

D                                              D*

D*  +  R                                  D- (semi or leuco) +  R+

At the platinum electrode, the semi/leuco form of the dye passes the electron to the platinum electrode, resulting in the formation of the original form of the dye.

D-                                       D   +     e-

Dark Chamber- The dye absorbs an electron from the SCE and transforms into the semi/leuco form. The leuco/semi form of the dye and the oxidized form of the reductant combine to produce the original dye and reductant molecules, repeating the process. The result is an electron stream that transforms light into electricity.

D   +     e-                                        D- (semi or leuco)

D-   +    R+                                       D   +   R

Fig- 1: Experimental setup of a Photogalvanic cell (Source- Ref.-2

Table 1: Different types of Dye-Surfactant-Reductant Systems were used in Photogalvanic cells.

III. CELL PARAMETERS

Dark potential (VDark): Initially, the whole system is placed in dark till it attains a stable potential. This stable potential is known as dark potential. It is represented by VDark and measured in V or mV.

Maximum potential (Vmax): After obtaining the dark potential, a rise in potential is seen when the platinum electrode is illuminated. The highest observed potential is known as maximum potential and represented by Vmax.

Open circuit voltage (Voc): The highest voltage that a solar cell can generate at zero current in the open circuit voltage. It is represented by Voc and measured in V or mV.

Photopotential (?V): The photopotential is calculated by the following mathematical expression

?V = Voc - VDark

Short circuit current (isc): The maximum current flowing through a solar cell when the voltage across it is zero (i.e. when the cell is short-circuited), is known as the short-circuit current. It is represented by isc and measured in A or mA.

Maximum current (imax): The photocurrent increased sharply in the first few minutes of illumination and it reaches a maximum value. This value is called maximum photocurrent. It is represented by imax.

Equilibrium current (ieq): After obtaining the maximum photocurrent, the current decreased slowly during the illumination and finally achieved a constant value. This photocurrent in its equilibrium condition is known as equilibrium photocurrent. It is represented by ieq.

Maximum power point (Ppp): The point at which the cell generates maximum electrical power. It is represented by Ppp and calculated by the following mathematical expression

Ppp= Vpp×ipp

Voltage at power point (Vpp): It is maximum potential at power point and represented by Vpp.

Current at power point (ipp): It is maximum current at power point and represented by ipp.

Fill Factor (FF): The fill factor is the most important parameter for evaluating the performance of solar cells. It is the ratio of maximum power to the product of short circuit current and open circuit voltage.

FF= PppVoc×isc= Vpp×ippVoc×isc

Conversion efficiency (CE): It is also the most important parameter of each cell, which represents the capability of a cell. It is the ratio of the electrical power output to input (incident energy from sunlight).

CE %=Vpp × ipp × FFP ×A ×100%

Storage capacity (t1/2): To determine the storage capacity of a photogalvanic cell, add an external load (current at power point) when illumination ends and the potential approaches a constant value. The storage capacity is determined in terms of t1/2, which is the time it takes for the output (power) to reduce by half at its power point in the dark. It can also be expressed as a percentage of charging time (charging time = tVmax - tVillum).

IV. CHALLENGES AND LIMITATIONS

One of the main challenges is improving efficiency, particularly addressing recombination losses that reduce overall energy conversion rates. Photogalvanic cells generally exhibit lower solar energy conversion efficiencies compared to traditional photovoltaic cells. This limits their widespread adoption for grid-scale power generation. The amount of energy a photogalvanic cell can store is directly related to the volume of the electrolyte solution. This limits their energy storage density compared to batteries. Maintaining the long-term stability and performance of photogalvanic cells can be challenging due to factors like electrolyte degradation and electrode corrosion. The cost of advanced materials and fabrication processes remains a barrier to the commercial scalability of PGCs.

V. FUTURE PROSPECTS

Research continues to improve the efficiency, storage capacity, and stability of Photogalvanic cells. Exploring new and more efficient photosensitizers with broader absorption spectra and longer excited state lifetimes is crucial Developing stable electrolytes with higher ionic conductivity and improved charge transport properties can enhance cell performance. Incorporating Nanomaterials like quantum dots or metal nanoparticles can enhance light absorption and charge separation processes. Focus on exploring novel reductant which are eco-friendly and cost-effective and that can efficiently regenerate the oxidized dye molecules in the Photogalvanic cell, improving overall cell performance and longevity.

Advances in materials science, particularly in the development of high-performance electrodes, electrolytes and Nanomaterials, have could further improve the efficiency and stability of Photogalvanic cells and   Photogalvanic cells could play a significant role in sustainable energy distribution.

Conclusion

Photogalvanic cells represent an exciting frontier in solar energy technology, merging conversion and storage capabilities in a single device. As the global energy landscape evolves, Photogalvanic cells are positioned as a promising technology that not only contributes to renewable energy generation but also supports the development of eco-friendly materials and systems. This review paper structure provides a comprehensive overview of Photogalvanic cells, covering materials, mechanisms, performance strategies, and future potential in the context of sustainable energy conversion. It would be suitable for researchers, students, and industry professionals interested in the latest developments and applications of this technology. Photogalvanic cells represent a promising avenue in the pursuit of sustainable energy technologies, with their unique mechanisms of energy conversion and storage. Continued advancements in this field may not only enhance their efficiency but also play a critical role in reducing reliance on fossil fuels and addressing global energy challenges. Research into their efficiency, materials, and long-term viability is ongoing, highlighting the need for further innovation in this field to optimize performance and scalability. As research continues to address their challenges and improve efficiency, these cells may play a crucial role in future sustainable energy systems, contributing to the global transition toward clean energy sources.

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