Abstract:
The dual functional materials can be formed by combining CO
2 adsorbent CaO with specific ethane oxidative dehydrogenation catalyst Cr/SBA−15 (mass ratio 1∶1) to achieve integrated CO
2 capture and utilization to produce ethylene. This study addresses the insufficient catalytic activity in dual functional materials by modifying Cr/SBA−15 through acid leaching, systematically investigating the effects of citric acid and nitric acid treatments on catalyst structure and performance. The catalysts with 3% Cr loading were synthesized by incipient wetness impregnation, followed by acid leaching at solid-liquid ratio 1∶20, 80℃ stirring for 4h. After washing and drying, the catalysts were mechanically mixed with CaO to prepare the dual functional material. Ultraviolet-visible spectroscopy results demonstrated that acid leaching enhanced Cr dispersion on the SBA−15 support surface. Microscopic surface morphology further confirmed uniform Cr distribution on the carrier. X-ray diffraction analysis revealed that acid treatment increased the proportion of Cr
6+ on the catalyst surface, promoting oxidation of Cr
3+ during calcination. N
2 adsorption-desorption tests showed that acid leaching enlarged the specific surface area and pore volume of the material. Solid state nuclear magnetic resonance results elucidated that acid leaching created framework vacancies by breaking Si-O bonds, enabling Cr anchoring to the carrier through silanol nests. Cr dispersion on the support depended on the availability of silanol nest hydroxyl groups, which were increased by acid treatment. Isothermal adsorption-catalysis experiments demonstrated significant performance improvement of the modified materials. Experimental results showed that after citric acid and nitric acid modifications, ethylene yield increased from 26% to 29% and 33% respectively, while ethane conversion rate improved from 37.19% to 47.17%. Combined catalyst characterization indicated that performance enhancement correlated with material property changes, where Cr valence state, dispersion degree, and specific surface area played crucial roles in catalytic activity improvement.