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3D Hierarchically Porous Nanostructured Catalyst Helps Efficiently Reduce CO2
- This new catalyst will bring CO2 one step closer to serving as a sustainable energy source. - KAIST researchers developed a three-dimensional (3D) hierarchically porous nanostructured catalyst with carbon dioxide (CO2) to carbon monoxide (CO) conversion rate up to 3.96 times higher than that of conventional nanoporous gold catalysts. This new catalyst helps overcome the existing limitations of the mass transport that has been a major cause of decreases in the CO2 conversion rate, holding a strong promise for the large-scale and cost-effective electrochemical conversion of CO2 into useful chemicals. As CO2 emissions increase and fossil fuels deplete globally, reducing and converting CO2 to clean energy electrochemically has attracted a great deal of attention as a promising technology. Especially due to the fact that the CO2 reduction reaction occurs competitively with hydrogen evolution reactions (HER) at similar redox potentials, the development of an efficient electrocatalyst for selective and robust CO2 reduction reactions has remained a key technological issue. Gold (Au) is one of the most commonly used catalysts in CO2 reduction reactions, but the high cost and scarcity of Au pose obstacles for mass commercial applications. The development of nanostructures has been extensively studied as a potential approach to improving the selectivity for target products and maximizing the number of active stable sites, thus enhancing the energy efficiency. However, the nanopores of the previously reported complex nanostructures were easily blocked by gaseous CO bubbles during aqueous reactions. The CO bubbles hindered mass transport of the reactants through the electrolyte, resulting in low CO2 conversion rates. In the study published in the Proceedings of the National Academy of Sciences of the USA (PNAS) on March 4, a research group at KAIST led by Professor Seokwoo Jeon and Professor Jihun Oh from the Department of Materials Science and Engineering designed a 3D hierarchically porous Au nanostructure with two different sizes of macropores and nanopores. The team used proximity-field nanopatterning (PnP) and electroplating techniques that are effective for fabricating the 3D well-ordered nanostructures. The proposed nanostructure, comprised of interconnected macroporous channels 200 to 300 nanometers (nm) wide and 10 nm nanopores, induces efficient mass transport through the interconnected macroporous channels as well as high selectivity by producing highly active stable sites from numerous nanopores. As a result, its electrodes show a high CO selectivity of 85.8% at a low overpotential of 0.264 V and efficient mass activity that is up to 3.96 times higher than that of de-alloyed nanoporous Au electrodes. “These results are expected to solve the problem of mass transfer in the field of similar electrochemical reactions and can be applied to a wide range of green energy applications for the efficient utilization of electrocatalysts,” said the researchers. This work was supported by the National Research Foundation (NRF) of Korea. Image credit: Professor Seokwoo Jeon and Professor Jihun Oh, KAIST Image usage restrictions: News organizations may use or redistribute this image, with proper attribution, as part of news coverage of this paper only. Publication: Hyun et al. (2020) Hierarchically porous Au nanostructures with interconnected channels for efficient mass transport in electrocatalytic CO2 reduction. Proceedings of the National Academy of Sciences of the USA (PNAS). Available online at https://doi.org/10.1073/pnas.1918837117 Profile: Seokwoo Jeon, PhD Professor firstname.lastname@example.org http://fdml.kaist.ac.kr Department of Materials Science and Engineering (MSE) https://www.kaist.ac.kr Korea Advanced Institute of Science and Technology (KAIST)Daejeon, Republic of Korea Profile: Jihun Oh, PhD Associate Professor email@example.com http://les.kaist.ac.kr Department of Materials Science and Engineering (MSE) Department of Energy, Environment, Water and Sustainability (EEWS) KAIST Profile: Gayea Hyun PhD Candidate firstname.lastname@example.org http://fdml.kaist.ac.kr Flexible Devices and Metamaterials Laboratory (FDML) Department of Materials Science and Engineering (MSE) KAIST Profile: Jun Tae Song, PhD Assistant Professor email@example.com http://www.cstf.kyushu-u.ac.jp/~ishihara-lab/ Department of Applied Chemistry https://www.kyushu-u.ac.jp Kyushu UniversityFukuoka, Japan (END)
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)
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