Hyo Sang Jeon

Achieving Selective and Efficient Electrocatalytic Activity for CO2 Reduction Using Immobilized Silver Nanoparticles

Selective electrochemical reduction of CO2 is one of the most sought-after processes because of the potential to convert a harmful greenhouse gas to a useful chemical. We have discovered that immobilized Ag nanoparticles supported on carbon exhibit enhanced Faradaic efficiency and a lower overpotential for selective reduction of CO2 to CO. These electrocatalysts were synthesized directly on the carbon support by a facile one-pot method using a cysteamine anchoring agent resulting in controlled monodispersed particle sizes. These synthesized Ag/C electrodes showed improved activities, specifically decrease of the overpotential by 300 mV at 1 mA/cm(2), and 4-fold enhanced CO Faradaic efficiency at -0.75 V vs RHE with the optimal particle size of 5 nm compared to polycrystalline Ag foil. DFT calculations enlightened that the specific interaction between Ag nanoparticle and the anchoring agents modified the catalyst surface to have a selectively higher affinity to the intermediate COOH over CO, which effectively lowers the overpotential.

Simple Chemical Solution Deposition of Co3O4 Thin Film Electrocatalyst for Oxygen Evolution Reaction

Oxygen evolution reaction (OER) is the key reaction in electrochemical processes, such as water splitting, metal-air batteries, and solar fuel production. Herein, we developed a facile chemical solution deposition method to prepare a highly active Co3O4 thin film electrode for OER, showing a low overpotential of 377 mV at 10 mA/cm(2) with good stability. An optimal loading of ethyl cellulose additive in a precursor solution was found to be essential for the morphology control and thus its electrocatalytic activity. Our results also show that the distribution of Co3O4 nanoparticle catalysts on the substrate is crucial in enhancing the inherent OER catalytic performance.

A monolithic and standalone solar-fuel device having comparable efficiency to photosynthesis in nature

The need for developing sustainable energy sources has generated academic and industrial attention in artificial photosynthesis, inspired by the natural process. In this study, we demonstrate a highly efficient solar energy to fuel conversion device using CO2 and water as feedstock. We developed a thin film photovoltaic technology for the light absorbing component using a low cost, solution based Cu(InxGa1−x)(SySe1−y)2 (CIGS) module fabrication method to provide sufficient potential for the conversion reactions. Our solar-fuel device uses cobalt oxide (Co3O4) nanoparticle thin film deposited with a low temperature coating method as the water oxidation catalyst and nanostructured gold film as the CO2 reduction to CO generation catalyst. We demonstrated that the integrated monolithic device operated by energy only from sunlight, in an absence of any external energy input. The individual components showed the following abilities: solar-to-power conversion efficiency of 8.58% for the CIGS photovoltaic module photoelectrode, overpotential reduction of water oxidation with the Co3O4 catalyst film by ∼360 mV at 5 mA cm−2, and Faradaic efficiency of over 90% by the nanostructured Au catalyst for CO2 reduction to CO. Remarkably, this is the first demonstration of a monolithic and standalone solar-fuel device whose solar-to-fuel conversion efficiency from CO2 and H2O is 4.23%, which is comparable with that of photosynthesis in nature.

Hydroxyapatite supported cobalt catalysts for hydrogen generation

The controlled generation of H(2) from storage materials by using an efficient catalytic support is a highly sought after technology; however, the majority of successes utilize expensive materials considered unfeasible. In our report on the creation of a novel, durable, and inexpensive catalytic support material for hydrogen generation, we examine a critical surface modification of hydroxyapatite (HAP) with cobalt ions to provide the necessary catalytic transition metal for the fast hydrolysis of the hydrogen storage material, sodium borohydride (NaBH(4)). By altering the morphology and composition of the HAP crystal supports, we revealed novel methods for enhancing the hydrogen generation rates. Particularly, lowering the Ca composition during synthesis of the HAP crystals afforded a Ca deficient HAP capable of exhibiting a higher surface coverage of cobalt, thereby eliciting faster hydrolysis reaction rates in comparison with the amorphous HAP control having the characteristic Ca content for HAP. A more significant increase in hydrogen generation was observed when using single crystal HAP in comparison with amorphous and calcium deficient HAP supports. Despite the smaller surface area of the hydrothermally prepared single crystal HAP, it provided significantly faster hydrogen generation. Each of the HAP supports exhibit repeatability with catalytic efficiency decreasing by approximately 25% over 3 weeks upon repeated daily exposure to solutions of the hydrogen storage material NaBH(4). Through these experiments, we proved that altering the composition and morphology of cobalt ion exchanged HAP supports can offers a useful means for increasing the rate of controlled hydrogen generation.

Chalcogenization-Derived Band Gap Grading in Solution-Processed CuInxGa1–x(Se,S)2 Thin-Film Solar Cells

Significant enhancement of solution-processed CuIn(x)Ga(1-x)(Se,S)2 (CIGSSe) thin-film solar cell performance was achieved by inducing a band gap gradient in the film thickness, which was triggered by the chalcogenization process. Specifically, after the preparation of an amorphous mixed oxide film of Cu, In, and Ga by a simple paste coating method chalcogenization under Se vapor, along with the flow of dilute H2S gas, resulted in the formation of CIGSSe films with graded composition distribution: S-rich top, In- and Se-rich middle, and Ga- and S-rich bottom. This uneven compositional distribution was confirmed to lead to a band gap gradient in the film, which may also be responsible for enhancement in the open circuit voltage and reduction in photocurrent loss, thus increasing the overall efficiency. The highest power conversion efficiency of 11.7% was achieved with J(sc) of 28.3 mA/cm(2), V(oc) of 601 mV, and FF of 68.6%.

Contributors to Enhanced CO2 Electroreduction Activity and Stability in a Nanostructured Au Electrocatalyst

The formation of a nanostructure is a popular strategy for catalyst applications because it can generate new surfaces that can significantly improve the catalytic activity and durability of the catalysts. However, the increase in the surface area resulting from nanostructuring does not fully explain the substantial improvement in the catalytic properties of the CO2 electroreduction reaction, and the underlying mechanisms have not yet been fully understood. Here, based on a combination of extended X-ray absorption fine structure analysis, X-ray photoelectron spectroscopy, and Kelvin probe force microscopy, we observed a contracted Au-Au bond length and low work function with the nanostructured Au surface that had enhanced catalytic activity for electrochemical CO2 reduction. The results may improve the understanding of the enhanced stability of the nanostructured Au electrode based on the resistance of cation adhesion during the CO2 reduction reaction.

Cocktails of Paste Coatings for Performance Enhancement of CuInGaS2 Thin-Film Solar Cells

To fabricate low-cost and printable wide-bandgap CuInxGa1-xS2 (CIGS) thin-film solar cells, a method based on a precursor solution was developed. In particular, under this method, multiple coatings with two pastes with different properties (e.g., viscosity) because of the different binder materials added were applied. Paste A could form a thin, dense layer enabling a high-efficiency solar cell but required several coating and drying cycles for the desired film thickness. On the other hand, paste B could easily form one-micrometer-thick films by means of a one-time spin-coating process but the porous microstructure limited the solar cell performance. Three different configurations of the CIGS films (A + B, B + A, and A + B + A) were realized by multiple coatings with the two pastes to find the optimal stacking configuration for a combination of the advantages of each paste. Solar cell devices using these films showed a notable difference in their photovoltaic characteristics. The bottom dense layer increased the minority carrier diffusion length and enhanced the short-circuit current. The top dense layer could suppress interface recombination but exhibited a low optical absorption, thereby decreasing the photocurrent. As a result, the A + B configuration could be suggested as a desirable simple stacking structure. The solar cell with A + B coating showed a highly improved efficiency (4.66%) compared to the cell with a film prepared by paste B only (2.90%), achieved by simple insertion of a single thin (200 nm), dense layer between the Mo back contact and a thick porous CIGS layer.

Surface modification of hydroxyapatite for hydrogen generation

Hydrogen provides a safe and clean alternative to carbon-based fuels. Having the proper catalytic support for production of hydrogen is a valuable technology. We report on the surface modification of hydroxyapatite as a novel catalytic support material for hydrogen generation. Aside from being inexpensive and durable, we reveal that Ru ion exchange on the HAP surface provides a highly active support for sodium borohydride hydrolysis, exemplifying a high total turnover number on the order of 24,000 mol H(2)/mol Ru. Moreover, we observe that the RuHAP support exhibits a long catalytic lifetime of approximately 1month upon repeated exposure to NaBH(4) solutions. We identified the ability of complex surface morphology to enhance hydrolysis by the catalytic transition metal covered surface. Particularly, we found that the complex morphology of polycrystalline RuHAP catalytic supports exhibits shorter induction times for hydrogen generation as well as improved reaction rates as compared with single crystal supports possessing the same Ru content. By decreasing induction time and enhancing catalytic activity, we find it feasible to further explore this catalyst support in the construction of a practical hydrogen generation system.

Semi-transparent thin film solar cells by a solution process

Easily processed, low cost, and highly efficient solar cells are desirable for photovoltaic conversion of solar energy to electricity. We present the fabrication of precursor solution processed CuInGaS2 (CIGS) thin film solar cells on transparent indium tin oxide (ITO) substrates. The CIGS absorber film was prepared by a spin-coating method, followed by two successive heat treatment processes. The first annealing process was on a hot plate at 300 °C for 30 min in air to remove carbon impurities in the film; this was followed by a sulfurization process at 500 °C in an H2S(1%)/Ar environment to form a polycrystalline CIGS film. The absorber film with an optical band-gap of 1.52 eV and a thickness of about 1.1 µm was successfully synthesized. Because of the usage of a transparent glass substrate, a bifacial CIGS thin film device could be achieved; its power conversion efficiency was measured to be 6.64% and 0.96% for front and rear illumination, respectively, under standard irradiation conditions.

A simple chemical route for composition graded Cu(In,Ga)S2 thin film solar cells: multi-stage paste coating

In order to realize the modulation of band-gap profile in low-cost and printable CuInxGa1−xS2 thin-film solar cells, a simple chemical route, namely a multi-stage paste coating method, was developed. In particular, with this method, multiple coatings with two precursor solution pastes with different compositions were applied. Elemental analysis techniques confirmed the formation of three different graded Ga distributions (front, back, and front-and-back gradient) throughout the absorber films depending on the coating sequence with two different pastes. The back gradient cell showed the largest power conversion efficiency of 7.29%, which was almost two times larger than those of the non-graded cells.