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Highly-Efficient Photoelectrochemical CO2 Reduction
Direct CO2 conversion has continuously attracted a great deal of attention as a technology to produce fuels and chemical building blocks from renewable energy resources. Specifically, substances such as carbon feedstocks and fuels can be produced by utilizing sunlight, water, and CO2 as semiconductors and a water interface through photoelectrochemical CO2 reduction. A KAIST research team demonstrated a novel photoelectrode structure for highly-selective and efficient photoelectrochemical CO2 reduction reactions. The research team led by Professor Jihun Oh of the Graduate School of EEWS (Energy, Environment, Water and Sustainability) presented a Si photoelectrode with a nanoporous Au thin film that is capable of reducing CO2 to CO with 90 percent selectivity in aqueous solution. The research team’s technology will provide a basic framework for designing the semiconductor photoelectrode structure necessary for photoelectrochemical conversion. In order to achieve steady conversion of CO2, it is necessary to use a high-performance catalyst to lower overpotential. Among the metal catalysts, Au is known to be an electrocatalyst that converts CO2 to CO. Conventionally, bare Au, as a catalyst, produces a lot of hydrogen gas due to its low CO selectivity. In addition, the high cost of Au remains a challenge in using the catalyst. Professor Oh’s research team addressed the issue by creating a nanoporous Au thin film formed by the electrochemical reduction of an anodized Au thin film. As a result, the team could demonstrate an efficient, selective photoelectrochemical reduction reaction of CO2 to CO using electrochemically-treated Au thin films on a Si photoelectrode. The electrochemical reduction on anodized Au thin films forms a nanoporous thin layer exhibiting many grain boundaries of nanoparticles on the Au surface. This dramatically improves the selectivity of the reduction reaction with a maximum CO faradaic efficiency of over 90% at low overpotential and durability. The research team also used an Au thin film of about 200 nanometers, 50,000 times thinner than previously reported nanostructured Au catalysts, resulting in a cost-effective catalyst. When depositing the catalyst on the semiconductor surface in the type of nanoparticles, the substrate of the thin film will be affected in the course of electrochemical reduction. Thus, the research team designed a new Si photoelectrode with mesh-type co-catalysts that are independently wired at the front and back of the photoelectrode without influencing the photoelectrode, and made it possible for electrochemical reduction. Due to the superior CO2 reduction reaction activity of the nanoporous Au mesh and high photovoltage from Si, the Si photoelectrode with the nanoporous Au thin film mesh shows conversion of CO2 to CO with 91% Faradaic efficiency at positive potential than CO equilibrium potential. Professor Oh explained, “This technology will serve as a platform for diverse semiconductors and catalysts. Researchers can further improve the solar-to-CO2 conversion efficiency using this technology. Dr. Jun Tae Song, the first author continued, “This new approach made it possible to develop a simple but very important type of electrode structure. It is the first time to achieve CO2 conversion at the potential lower than equilibrium potential. We believe that our research will contribute to efficient CO2 conversion.” This research was published in the inside front cover of Advanced Energy Materials on February 8, 2017. The research was funded and supported by the Korea Carbon Capture & Sequestration R&D Center. Professor Sung-Yoon Chung of the EEWS also participated in this research. (Figure: Schematic diagram of a Si photoelectrode that patterns with mesh-type nanoporous Au)
KAIST Team Develops Semi-Transparent Solar Cells with Thermal Mirror Capability
A research team led by KAIST and Sungkyunkwan University professors has created semi-transparent perovskite solar cells that demonstrate high-power conversion efficiency and transmit visible light while blocking infrared light, making them great candidates for solar windows. Modern architects prefer to build exteriors designed with glass mainly from artistic or cost perspectives. Scientists, however, go one step further and see opportunities from its potential ability to harness solar energy. Researchers have thus explored ways to make solar cells transparent or semi-transparent as a substitute material for glass, but this has proven to be a challenging task because solar cells need to absorb sunlight to generate electricity, and when they are transparent, it reduces their energy efficiency. Typical solar cells today are made of crystalline silicon, but it is difficult to make them translucent. Semi-transparent solar cells under development use, for example, organic or dye-sensitized materials, but compared to crystalline silicon-based cells, their power-conversion efficiencies are relatively low. Perovskites are hybrid organic-inorganic halide-based photovoltaic materials, which are cheap to produce and easy to manufacture. They have recently received much attention as the efficiency of perovskite solar cells has rapidly increased to the level of silicon technologies in the past few years. Using perovskites, a Korean research team led by Professor Seunghyup Yoo of the Electrical Engineering School at KAIST and Professor Nam-Gyu Park of the Chemical Engineering School at Sungkyunkwan University developed a semi-transparent solar cell that is highly efficient and, additionally, functions very effectively as a thermal-mirror. The team has developed a top transparent electrode (TTE) that works well with perovskite solar cells. In most cases, a key to success in realizing semi-transparent solar cells is to find a TTE that is compatible with a given photoactive material system, which is also the case for perovskite solar cells. The proposed TTE is based on a multilayer stack consisting of a metal film sandwiched between a high refractive-index (high-index) layer and an interfacial buffer layer. This TTE, placed as a top-most layer, can be prepared without damaging ingredients used in perovskite solar cells. Unlike conventional transparent electrodes focusing only on transmitting visible light, the proposed TTE plays the dual role of passing through visible light while reflecting infrared rays. The semi-transparent solar cells made with the proposed TTEs exhibited average power conversion efficiency as high as 13.3% with 85.5% infrared rejection. The team believes that if the semi-transparent perovskite solar cells are scaled up for practical applications, they can be used in solar windows for buildings and automobiles, which not only generate electrical energy but also enable the smart heat management for indoor environments, thereby utilizing solar energy more efficiently and effectively. This result was published as a cover article in the July 20, 2016 issue of Advanced Energy Materials. The research paper is entitled “Empowering Semi-transparent Solar Cells with Thermal-mirror Functionality.” (DOI: 10.1002/aenm.201502466) The team designed the transparent electrode (TE) stack in three layers: A thin-film of silver (Ag) is placed in between the bottom interfacial layer of molybdenum trioxide (MoO3) and the top high-index dielectric layer of zinc sulfide (ZnS). Such a tri-layer approach has been known as a means to increase the overall visible-light transmittance of metallic thin films via index matching technique, which is essentially the same technique used for anti-reflection coating of glasses except that the present case involves a metallic layer. Traditionally, when a TE is based on a metal film, such as Ag, the film should be extremely thin, e.g., 7-12 nanometers (nm), to obtain transparency and, accordingly, to transmit visible light. However, the team took a different approach in this research. They made the Ag TE two or three times thicker (12-24 nm) than conventional metal films and, as a result, it reflected more infrared light. The high refractive index of the ZnS layer plays an essential role in keeping the visible light transmittance of the proposed TTE high even with the relatively thick Ag film when its thickness is carefully optimized for maximal destructive interference, leading to low reflectance (and thus high transmittance) within its visible light range. The team confirmed the semi-transparent perovskite solar cell’s thermal-mirror function through an experiment in which a halogen lamp illuminated an object for five minutes through three mediums: a window of bare glass, automotive tinting film, and the proposed semi-transparent perovskite solar cell. An infrared (IR) camera took thermal images of the object as well as that of each window’s surface. The object’s temperature, when exposed through the glass window, rose to 36.8 Celsius degrees whereas both the tinting film and the cell allowed the object to remain below 27 Celsius degrees. The tinting film absorbs light to block solar energy, so the film’s surface became hot as it was continuously exposed to the lamp light, but the proposed semi-transparent solar cell stayed cool since it rejects solar heat energy by reflection, rather than by absorption. The total solar energy rejection (TSER) of the proposed cell was as high as 89.6%. Professor Yoo of KAIST said, “The major contributions of this work are to find transparent electrode technology suitable for translucent perovskite cells and to provide a design approach to fully harness the potential it can further deliver as a heat mirror in addition to its main role as an electrode. The present work can be further fine-tuned to include colored solar cells and to incorporate flexible or rollable form factors, as they will allow for greater design freedom and thus offer more opportunities for them to be integrated into real-world objects and structures such as cars, buildings, and houses.” The lead authors are Hoyeon Kim and Jaewon Ha, both Ph.D. candidates in the School of Electrical Engineering at KAIST, and Hui-Seon Kim, a student in the School of Chemical Engineering at Sungkyunkwan University. This research was supported mainly by the Climate Change Research Hub Program of KAIST. Picture 1: Semi-transparent Perovskite Solar Cell This picture shows a prototype of a semi-transparent perovskite solar cell with thermal-mirror functionality. Picture 2: A Heat Rejection Performance Comparison Experiment This picture presents thermal images taken by an infrared camera for comparing the heat rejection performance of bare glass, automotive tinting film, and a semi-transparent perovskite solar cell after being illuminated by a halogen lamp for five minutes.
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