Modification of Copper Benzene-1,3,5-tricarboxy Late (Cu-BTC) Composites with Multiwalled Carbon Nanotubes and Amino Groups for Enhanced CO2/CH4 Selective Adsorption Performance and Water Stability

CNT-NH2-Cu-BTC was prepared via hydrothermal synthesis for the adsorption and separation of CO2/CH4 mixtures with 2, 6, and 10% multiwalled carbon nanotube (MWCNT) additions. NH2-BTC composites were synthesized by changing the organic ligand and adding NH2-BDC (15, 25, 35, and 45%) to improve the adsorption capacity. MWCNTS were loaded to enhance the water stability of the material. The structure, surface morphology, and pore size distribution of the composites were characterized using X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, thermogravimetric analysis, and specific surface area and pore structure measurements. The CO2/CH4 selective adsorption performance was studied via breakthrough experiments using a self-made adsorption device. The CO2 adsorption capacity of Cu-BTC increased due to the addition of NH2-BDC, with 35%NH2-Cu-BTC exhibiting the best CO2 adsorption property, i.e., a CO2 adsorption capacity of 1.82 mmol/g and a CO2/CH4 separation coefficient of 1.44 at 35 °C and 20 mL/min. After adding MWCNTs, 6%CNT-NH2-Cu-BTC exhibited the best CO2 adsorption property and water stability, with the CO2 adsorption capacity increasing to 2.06 mmol/g. 6%CNT-NH2-Cu-BTC with wet impregnation retained 79% of the CO2 adsorption capacity of the sample without wet impregnation, demonstrating its excellent water stability under humid conditions. Cyclic experiments with and without wet impregnation were performed.