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16. Optimization of Cu/MnO2 catalyst for enhanced methane bi-reforming: a response surface methodology approach for sustainable syngas production.

Author

Ibrahim, Irna Haslina, Shafiqah, Mohd-Nasir Nor, Suhaimi, Nuremirah Syafiqah, Li, Maoshuai, Van Cuong, Nguyen, and Zainal Abidin, Sumaiya

Subjects
SUSTAINABILITY, ENERGY shortages, X-ray diffraction, ANALYSIS of variance, ENERGY futures
Abstract

Hydrogen or syngas, valued for its clean and high-energy properties, stands as a promising solution to future energy shortages by converting CO2 and CH4 waste into renewable syngas through a reaction known as methane bi-reforming. Hence, the purpose of this current research is to examine the effectiveness of Cu/MnO2 catalyst in methane bi-reforming (MBR) using response surface methodology (RSM). The synthesis of the 15%Cu/MnO2 catalyst was accomplished using the ultrasonic impregnation method, followed by a comprehensive analysis and characterization of the catalyst using CO2-TPD, BET, H2-TPR, TPO, and XRD evaluation. The effect of reaction parameters was investigated using RSM analysis, including temperature, CO2/CH4 ratio, and gas hourly space velocity (GHSV) (700–900 °C, 0.2–1.0, and 16–36 L g cat−1 h−1, respectively). According to the analysis of variance and three-dimensional response surface plots, it was determined that CH4 conversion and H2 yield were largely influenced by temperature, whereas CO2 conversion and CO yield could be manipulated through CO2/CH4 feed ratio. Meanwhile, the GHSV appeared to have a significant influence on the H2/CO ratio and CH4 conversion. From the experimental data, it was found that the 15%Cu/MnO2 catalyst performed best under specified optimal conditions of 800 °C, a CO2/CH4 ratio of 0.6, and a GHSV of 26 L g cat−1 h−1. These optimal conditions resulted in the maximum conversion of CH4 (54.67%), CO2 conversion (47.52%), H2 yield (43.81%), CO yield (36.29%), and H2/CO ratio (1.384). Despite the inevitability of carbon formation resulting from the breakdown of CH4 and CO at high temperatures, the examination of the spent catalysts under optimal conditions yielded a smaller quantity of carbon of approximately 28.27% in comparison to the suboptimal conditions with 55.37%. [ABSTRACT FROM AUTHOR]

Published
2024
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20. Development of gold and copper catalysts for sustainable chemical processing

Author

Li, Maoshuai and Keane, Mark A.

Subjects
660
Abstract

Supported Au and Cu catalysts have been developed for clean/sustainable production of value fine chemicals (including alcohols, ketone, amines and imines) from selective reduction (of benzaldehyde, nitrobenzene and furfural) and coupled (dehydrogenation-hydrogenation) reaction in the continuous gas phase operation. Critical catalyst physicochemical properties are characterised by applying a range of techniques and correlated to the catalytic response. The role of support, Au particle size and electronic character in determining catalytic activity and selectivity in the hydrogenation of benzaldehyde and nitrobenzene over oxide supported nano-scale (2-8 nm) Au has been established. Hydrogenation (turnover frequency) TOF increases with decreasing Au size (from 8 to 4 nm) with measurably lower TOF over Au < 3 nm. Repulsion of –C=O and –NO2 functionalities with respect to Auδ+ and strong binding to surface oxygen vacancies have been found to lower hydrogenation rates. Promotional effect of water via catalytic dissociation has been found to enhance the selective benzaldehyde hydrogenation rate. Two catalytic routes for imine (N-benzylideneimine) synthesis in continuous gas phase operation have been established. Reductive coupling of benzaldehyde with nitrobenzene (using external hydrogen) over supported Au generated up to 99% selectivity to the target imine. Coupling of benzyl alcohol dehydrogenation with nitrobenzene hydrogenation (in the absence of external hydrogen supply) over Au/TiO2 + Cu/SiO2 mixture produced imine with full hydrogen utilisation. Incorporation of Au/TiO2 to Cu/SiO2 created a synergy between Cu and Au and enhanced catalyst stability. A tandem dehydrogenation/amination/reduction process has been developed for high throughout production of benzylamine in continuous gas phase operation over Cu/SiO2 and Au/TiO2. A synergy between Cu/SiO2 and Au/TiO2 serves to promote benzylamine formation with 81% yield achieved through an optimization of process parameters. Coupling of 2-butanol dehydrogenation with nitrobenzene hydrogenation over Cu/SiO2 in the absence of an external H2 supply delivered exclusive production of both 2-butanone and aniline at full conversion. Hydrogen utilisation efficiency was appreciably greater (by a factor of up to 50) in the coupled system relative to conventional stand-alone hydrogenation using pressurised hydrogen. Selective conversion of biomass-derived furfural to furfuryl alcohol over supported Au catalysts has been established. A series of approaches (e.g. promotional effect of water via catalytic dissociation, increased spillover hydrogen with addition of oxide support and coupling strategy) directed at increasing the surface availability of reactive hydrogen were adopted to enhance furfuryl alcohol production and hydrogen utilisation. Continuous production of γ-butyrolactone has been established in both stand-alone hydrogenation of succinic acid (using external H2) and reaction coupling with formic acid decomposition (as a source of H2) over Cu/SiO2. Pd/SiO2 and Ni/SiO2 promoted propanoic acid formation at higher reaction rates. The results presented in this thesis establish feasible catalytic routes to high value alcohols, imines and amines where critical process optimisation is demonstrated in terms of catalyst composition/surface structure and reaction conditions.

Published
2016

31. Contributors

Author

Belenkaya, Irina V., primary, Belyaev, Vladimir D., additional, Bespalko, Yulia N., additional, Bobrova, Lyudmila N., additional, Bokarev, Dmitry A., additional, Bolotov, Vladimir A., additional, Bragina, Olga A., additional, Bukhtiyarov, Valerii I., additional, Cortés Corberán, V., additional, Dutov, Valery V., additional, Eremeev, Nikita F., additional, Fedorova, Yulia E., additional, Galvita, Vladimir V., additional, Golubina, Elena V., additional, Gurevich, Sergey A., additional, Hu, Guannan, additional, Jose, Nicholas, additional, Kharlamova, Tamara S., additional, Korobeynikov, Mikhail V., additional, Kozhevin, Vladimir M., additional, Kozlova, Ekaterina A., additional, Krasnov, Alexey V., additional, Krieger, Tamara A., additional, Lapkin, Alexei, additional, Li, Changdong, additional, Li, Maoshuai, additional, Lokteva, Ekaterina S., additional, Lukashevich, Anton I., additional, Mamontov, Grigory V., additional, Marin, Guy B., additional, Maslakov, Konstantin I., additional, Mateyshina, Yulia G., additional, Mezentseva, Natalia V., additional, Mikhailenko, Mikhail A., additional, Murzin, Dmitry Yu., additional, Nemudry, Alexander P., additional, Parmon, Valentin N., additional, Poelman, Hilde, additional, Prosvirin, Igor P., additional, Rebrov, Evgeny, additional, Rives, V., additional, Rostovshchikova, Tatiana N., additional, Sadovskaya, Ekaterina M., additional, Sadykov, Vladislav A., additional, Salaev, Mikhail A., additional, Shmakov, Alexander N., additional, Simakova, Irina L., additional, Skriabin, Pavel I., additional, Smorygo, Oleg L., additional, Stakheev, Alexandr Yu., additional, Stathopoulos, V., additional, Tanashev, Yuri Yu., additional, Theofanidis, Stavros Alexandros, additional, Ulihin, Artem S., additional, Uvarov, Nikolai F., additional, van Veen, Andre C., additional, Vinokurov, Zakhar S., additional, Vodyankina, Olga V., additional, and Yavsin, Denis A., additional

Published
2019
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35. An Insight into Synergistic Metal-Oxide Interaction in CO 2 Hydrogenation to Methanol over Cu/ZnO/ZrO 2.

Author

Chang, Xiao, Zi, Xiaohui, Li, Jing, Liu, Fengdong, Han, Xiaoyu, Chen, Jiyi, Hao, Ziwen, Zhang, Heng, Zhang, Zhenmei, Gao, Pengju, Li, Maoshuai, Lv, Jing, and Ma, Xinbin

Subjects
COPPER, CARBON dioxide, HYDROGENATION, CATALYST structure, ZINC oxide, METHANOL, METHANOL as fuel
Abstract

The metal-oxide interaction is of significance to the construction of active sites for Cu-catalyzed CO2 hydrogenation to methanol. This study examines the effect of ZnO and ZrO2 composition on the Cu/ZnO/ZrO2 catalyst structure and surface properties to further tune the catalytic activity for methanol synthesis. The ZnO/ZrO2 ratio can impact the CuZn alloy formation from strong Cu-ZnO interactions and the surface basic sites for CO2 adsorption at the Cu-ZrO2 interface. The proportional correlation of the CuZn alloy content and CO2 desorption amount with the space-time yield (STY) of methanol reveals a synergistic interaction between Cu and oxides (ZnO and ZrO2) that enhances methanol synthesis. The optimized Cu/ZnO/ZrO2 catalyst exhibits higher STY relative to the traditional Cu/ZnO/Al2O3 catalyst. The obtained results presented herein can provide insight into the catalyst design for methanol synthesis from CO2. [ABSTRACT FROM AUTHOR]

Published
2023
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