The development of efficient catalyst materials that can drive high catalytic performance is challenging. Here, we report a well-defined hollow mesoporous TiN nanostructure for use as Pt catalyst support material for methanol electro-oxidation. The hollow TiN nanostructure was synthesized by the ammonia nitridation of pre-synthesized mother hollow anatase TiO2, which was prepared by SiO2 template-assisted sol–gel synthesis followed by chemical etching, acid treatment, and sequential calcination. The variation in the ammonia nitridation temperature allowed the crystalline properties of the samples to be finely tuned. As the ammonia nitrification temperature increased, the crystallinity of the resulting hollow TiN continuously increased, and the corresponding Pt catalysts showed enhanced activity toward methanol electro-oxidation. The hollow TiN-800 sample (H-TiN-800), with a well-developed pure TiN phase, exhibited the highest electrical conductivity and the lowest resistance. The corresponding Pt/H-TiN-800 catalyst exhibited significantly enhanced catalytic activity. In this study, we systemically analyzed the physicochemical characteristics and electrochemical performance of hollow TiN samples and their corresponding Pt catalysts.
The development of an efficient and economic catalyst with high catalytic performance is always challenging. In this study, we report the synthesis of hollow CeO2 nanostructures and the crystallinity control of a CeO2 layer used as a support material for a CuO-CeO2 catalyst in CO oxidation. The hollow CeO2 nanostructures were synthesized using a simple hydrothermal method. The crystallinity of the hollow CeO2 shell layer was controlled through thermal treatment at various temperatures. The crystallinity of hollow CeO2 was enhanced by increasing the calcination temperature, but both porosity and surface area decreased, showing an opposite trend to that of crystallinity. The crystallinity of hollow CeO2 significantly influenced both the characteristics and the catalytic performance of the corresponding hollow CuO-CeO2 (H-Cu-CeO2) catalysts. The degree of oxygen vacancy significantly decreased with the calcination temperature. H-Cu-CeO2 (HT), which presented the lowest CeO2 crystallinity, not only had a high degree of oxygen vacancy but also showed well-dispersed CuO species, while H-Cu-CeO2 (800), with well-developed crystallinity, showed low CuO dispersion. The H-Cu-CeO2 (HT) catalyst exhibited significantly enhanced catalytic activity and stability. In this study, we systemically analyzed the characteristics and catalyst performance of hollow CeO2 samples and the corresponding hollow CuO-CeO2 catalysts.
The effects of operating parameters such as reaction temperature, space velocity, and feed gas composition on the performance of the methane dry-reforming reaction (DRM) over the Ni/Al2O3 catalyst are systemically investigated. The Ni/Al2O3 catalyst, which is synthesized by conventional wet impregnation, showed well-developed mesoporosity with well-dispersed Ni nanoparticles. CH4 and CO2 conversions over the Ni/Al2O3 catalyst are dramatically increased as both the reaction temperature is increased, and space velocity is decreased. The feed gas composition, especially the CO2/CH4 ratio, significantly influences the DRM performance, catalyst deactivation and the reaction behavior of side reactions. When the CO2-rich gas composition (CO2/CH4 > 1) was used, a reverse water gas shift (RWGS) reaction significantly occurred, leading to the consumption of hydrogen produced from DRM. The CH4-rich gas composition (CO2/CH4 < 1) induces severe carbon depositions followed by a reverse Boudouard reaction, resulting in catalytic activity drastically decreasing at the beginning followed by a stable conversion. The catalyst after the DRM reaction with a different feed ratio was analyzed to investigate the amount and structure of carbon deposited on the catalyst. In this study, we suggested that the optimal DRM reaction conditions can achieve stable performances in terms of conversion, hydrogen production and long-term stability.
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